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Attosecond physics phenomena at nanometric tips M F Ciappina, J A Pérez-Hernández, A S
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M Krüger, M Schenk, M Förster et al.

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J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001 (33pp) https://doi.org/10.1088/1361-6455/aac6ac

Topical Review

Attosecond physics phenomena at

nanometric tips
Michael Krüger1,5 , Christoph Lemell2 , Georg Wachter2,
Joachim Burgdörfer2 and Peter Hommelhoff3,4
1
Department of Physics of Complex Systems, Weizmann Institute of Science, 234 Herzl Street, Rehovot
76100, Israel
2
Institute for Theoretical Physics, Wiedner Hauptstraße 8-10, Vienna University of Technology, 1040
Vienna, Austria
3
Department of Physics, Friedrich-Alexander-Universität Erlangen-Nürnberg (FAU), Staudtstraße 1,
91058 Erlangen, Germany
4
Max-Planck-Institut für die Physik des Lichts, Staudtstraße 2, 91058 Erlangen, Germany

E-mail: michael.krueger@weizmann.ac.il, lemell@concord.itp.tuwien.ac.at and peter.hommelhoff@

physik.uni-erlangen.de

Received 16 February 2018, revised 15 April 2018

Accepted for publication 22 May 2018
Published 9 August 2018

Abstract
Attosecond science is based on electron dynamics driven by a strong optical electric field and has
evolved beyond its original scope in gas-phase atomic and molecular physics to solid-state targets. In
this review, we discuss a nanoscale attosecond physics laboratory that has enabled the first
observations of strong-field-driven photoemission and recollision at a solid surface: laser-triggered
metallic nanotips. In addition to the research questions of rather fundamental nature, femtosecond
electron sources with outstanding beam qualities have resulted from this research, which has prompted
follow-up application in the sensing of electric fields and lightwave electronics, ultrafast microscopy
and diffraction, and fundamental matter-wave quantum optics. We review the theoretical and
experimental concepts underlying near-field enhancement, photoemission regimes and electron
acceleration mechanisms. Nanotips add new degrees of freedom to well known strong-field
phenomena from atomic physics. For example, they enable the realization of a true sub-optical-cycle
acceleration regime where recollision is suppressed. We also discuss the possibility of high-harmonic
generation due to laser irradiation of metallic nanostructures.

Keywords: Attosecond physics, nano-optics, strong-field physics

(Some figures may appear in colour only in the online journal)

1. Introduction and early developments
The discovery of the surprisingly efficient generation of high-
harmonic radiation from atomic gases (McPherson et al 1987,
5
Author to whom any correspondence should be addressed.
Original content from this work may be used under the terms
of the Creative Commons Attribution 3.0 licence. Any
further distribution of this work must maintain attribution to the author(s) and
the title of the work, journal citation and DOI.
Ferray et al 1988) has led to the invention and broad accep-
tance of the recollision picture, which is at the core of the so-
called simple man’s model or three-step model. While its
origins date back about 30 years (Kuchiev 1987, Galla-
gher 1988, van Linden and van den Heuvell 1988), the model
was widely accepted about 25 years ago when a number of
papers appeared (Corkum 1993, Schafer et al 1993, Becker
et al 1995). It is thus appropriate to celebrate the 25th anni-
versary of the recollision picture with this special issue. Since
then, several new and quite spectacular research fields have
grown out of the initial discoveries, which originated in the

0953-4075/18/172001+33$33.00 1 © 2018 IOP Publishing Ltd Printed in the UK

J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001
realm of high-field atomic physics but have now reached out
into various other disciplines (see Calegari et al (2016) for an
overview of recent developments). Examples include the
efficient generation of coherent extreme ultraviolet (XUV)
and even x-ray pulses, the generation of attosecond light
pulses, electron diffraction experiments with the electrons
emitted from the irradiated atoms, molecules and clusters, and
strong-field and recollision physics in condensed matter. In
this contribution, we provide a review on this last topic,
namely strong-field and recollision physics at the surface of
nanoscale solids. Aspects of this research are reflected in a
number of reviews and books (Vasa et al 2009, Krüger
et al 2012a, Hommelhoff and Kling 2015, Jones et al 2016,
Ciappina et al 2017). The focus of our review will be on a
particular nanostructure geometry: sharp metallic needle tips.
We will recapitulate how three well-established fields
came together to merge into a new field, offering new insight
and applications alike: (1) a century of experience in field
emission from needle tips, (2) atomic recollision physics, and
(3) nano-optics, also known as near-field optics. This com-
bination enables an unprecedented confinement of light–
matter interaction to nanometer length and attosecond time
scales.
1.1. Overview and structure
In the following part of the introduction (section 1.2), we will
review early work on needle tips and strong-field photo-
emission from solids. Because nano-optics is of high impor-
tance for strong-field physics at needle tips, we will discuss it
in greater detail in Chapter 2. Chapter 3 deals with exper-
imental methods that have been used to elucidate the many
open questions around the merger of gas-phase strong-field
physics with solid-state systems. In Chapter 4, we discuss
photoemission mechanisms, the in-depth understanding of
which is not only important in its own right but for realizing
new ultrafast and coherent electron sources. In Chapter 5, an
overview is given of theoretical methods that are frequently
used for the modeling of strong-field physics at metal tips.
Temporal dynamics of the emission processes is discussed in
more detail in Chapter 6, while prototypical strong-field
effects, namely the acceleration and recollision of photo-
electrons by the waveform of the driver field, are reviewed in
Chapter 7. Modulating the waveform enables the control of
strong-field photoemission and acceleration, as discussed in
Chapter 8. Chapter 9 explores the feasibility of high-harmonic
generation (HHG) at nanotips and presents the first ab initio
results. In Chapter 10, we give a brief overview of the wide
range of applications of the observed strong-field phenomena
at needle tips, before concluding our review in Chapter 11.
1.2. Early work
Sharp metal needle tips have already been used for more than
80 years, even before the pioneering works of Erwin W
Müller (Müller 1936), as excellent electron sources in various
applications. The electron beam emitted from such a tip, in
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Topical Review
particular in cold field emission mode, is extremely bright and
coherent, which is the reason it is routinely used in high-
resolution electron microscopes, even though the easier-to-
operate Schottky sources are nowadays preferred despite their
slightly inferior performance (Spence 2013). A highly
coherent electron beam can be generated in DC operation
when a strong static negative electric field is applied to a
metal tip. Because of the accumulation of field lines at the tip
apex, the potential landscape in the vicinity of the apex is
changed so that electrons can tunnel through the potential
barrier from the metal to the vacuum side. This is the well
known field emission process, requiring static field strengths
in excess of 1 GV m−1 to observe a measurable electron
current from a typical metal.
Nonlinear photoemission, in particular the two con-
ceptually identical processes of above-threshold ionization of
atoms and above-threshold photoemission from solids,
represents the foundation on which strong-field physics
stands. We recall early work on laser-driven (multi-) photon–
electron emission from solids, before we go in medias res.
With ‘early’ we refer to work published before the three
2006/2007 papers, which can be considered the first report on
coherent electron sources driven by ultrafast photoemission
processes (Hommelhoff et al 2006b, 2006c, Ropers et al
2007c). Subsequent papers provided clear evidence of strong-
field physics at metal tips (Bormann et al 2010, Schenk
et al 2010).
Multiphoton photoemission from metals dates back to the
seminal work by Keldysh in 1965 (Keldysh 1965). In the
same year, Keldysh’s method was applied to metals by
Bunkin and Fedorov, who, in essence, showed that the lim-
iting cases are DC field emission in the low-frequency limit
and multiphoton physics for high frequencies (Bunkin and
Fedorov 1965), closely mirroring analogous concepts in
atomic physics.
On the experimental side, the invention of the laser
quickly led to the discovery of nonlinear photoemission; two-
photon photoemission from solids was first observed in 1964
at a semiconducting Cs3Sb photocathode (Sonnenberg
et al 1964). In Budapest, Farkas and colleagues investigated
higher-order nonlinear photoemission early on with pico-
seond laser pulses (Farkas et al 1971, 1972, Farkas and
Chin 1985), referring to Keldysh’s theoretical work. Clear
deviations from perturbative multiphoton emission and the
onset of optical tunneling effects in electron emission from a
gold surface were reported in 1991 (Tóth et al 1991).
In parallel, the photofield emission process was investi-
gated and later utilized for inferring the band structure of metals.
Here, an electron is photo-excited inside the metal close to or
below the emission threshold, and then undergoes field emis-
sion (Lee 1973, Radoń 1998). Because field emission is
exponentially sensitive to the barrier height, a current mea-
surement as a function of the applied DC voltage allows the
identification of the origin of the electrons; this, in combination
with the known but variable photon energy, enables a recon-
struction of the band structure of the metal under scrutiny.
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001
While the well-defined excitation of electrons (from close
to the Fermi level) to a well-defined intermediate state is the
basis of photofield emission spectroscopy, the (laser-pulse-
induced) heating of the electron gas inside a metal tip also
leads to enhanced electron emission rates (Lee et al 1980,
Riffe et al 1993). Hence, spectral information of the emitted
electrons is mandatory to obtain a clear picture of the emis-
sion process and its dynamics. In particular, the question
arises whether the participating electrons thermalize before
they are emitted, or whether the electrons are emitted coher-
ently as indicated by photon orders showing up in the spectra.
However, an unstructured spectrum does not necessarily
imply that the emission is thermal and incoherent, as photo-
emission studies from flat metals are prone to focal averaging
effects. Focal averaging implies that electrons emitted in
various regions of the laser spot experience different peak
laser field strengths leading to a smeared-out electron energy
distribution, to the extent that photon orders are no longer
discernible. Yet another effect often arising in photoemission
in the high-intensity regime from flat metal surfaces can wash
out photon orders, namely space-charge repulsion within the
emitted electron cloud. The reader is referred to earlier work
on flat metal surfaces, for example, to Aeschlimann et al
(1995), Damascelli et al (1996), and to Gault et al (2007),
Kealhofer et al (2012) for more recent work on metal nee-
dle tips.
Two-photon photoemission (2PPE), in particular time-
resolved 2PPE, is the method of choice for inferring various
(often electronic) time scales in metals. It has strong ties to
strong-field physics at metal surfaces, given the fact that this
method allows the measurement of electronic processes on
the femtosecond scale. We will not discuss this broad research
field further, but refer the reader to two reviews (Petek and
Ogawa 1997, Bauer et al 2015).
Laser pulses with sub-picosecond duration are necessary
for these studies to reach the nonlinear photoemission regime
without inducing damage to the sample. The large deviation
of the electron temperature from the lattice temperature on
sub-picosecond time scales is indeed important for explaining
the observed emission behavior in photoemission experiments
with sub-picosecond pulses (Riffe et al 1993, Girardeau-
Montaut and Girardeau-Montaut 1995).
Long before the recollision picture had been introduced,
above-threshold ionization had been observed from atoms
(Agostini et al 1979, Kruit et al 1981), where many photon
orders could be unequivocally identified in photoionization
spectra. Similarly, shifting of the multiphoton peaks because
of field effects, in particular the AC Stark effect and the role
of the ponderomotive potential, had been well understood
through experiments from atoms in the gas phase (Kruit
et al 1983, Muller et al 1983, Bucksbaum et al 1987). Some
ten years later, indications of the counterparts in photoemis-
sion from solids had been reported: above-threshold photo-
emission (ATP) including potential ponderomotive effects
initially in the late 80s (Luan et al 1989, Fann et al 1991,
Farkas et al 1993) and later more clearly (Banfi et al 2005,
Bisio et al 2006). Notably, well-defined photon orders could
be observed, and the prevalence of prompt coherent emission
3
Topical Review
over thermionic emission was made possible by excitation
with laser pulses with a duration below 200 fs (Ferrini
et al 2009).
Around the year 2000, the invention of the frequency
comb allowed control of the optical carrier field within the
laser-pulse envelope (Udem et al 1999, Diddams et al 2000,
Jones et al 2000, Udem et al 2002, Hänsch 2006). This was
enabled by controlling the relative phase between the carrier
field maximum and pulse envelope maximum, the carrier-
envelope offset phase, or, in short, carrier-envelope phase
(CEP). In the strong-field regime with atoms, it allowed full
control over the electron dynamics on attosecond time scales
and the generation of isolated attosecond XUV light pulses
(Baltuška et al 2003, Kienberger et al 2004, Sansone
et al 2006). Lemell et al (2003) performed a numerical
investigation of the CEP dependence of the electron emission
current from a metal surface based on a jellium model. They
predicted a significant CEP-dependent current for various
intensity regimes, in particular for low intensities in the
intermediate regime between multiphoton and tunneling
photoemission. Apolonski et al (2004) indeed observed a
CEP-dependent current contribution from a flat metal surface
illuminated with sub-two cycle laser pulses, but it was found
to be very small. In theoretical studies, Faisal et al (2005)
predicted electron emission spectra from solid surfaces that
bear reminiscence of the hallmark high-harmonic plateau well
known from atomic physics. They indeed relate their num-
erical observations to the recollision plateau in atomic physics
—the first study to note that recollision of electrons might
appear at a metal surface.
Around the same time spectrally resolved experiments
were performed on electron emission from flat metal surfaces
with femtosecond laser pulses, revealing above-threshold
photon orders, i.e. electrons emitted with kinetic energies
larger than at least the energy of a driving-laser photon (Banfi
et al 2005, Bisio et al 2006). The observation of above-
threshold orders represents the first step towards observing
the exciting physics involving electrons with energies much
higher than needed just for their emission from the solid,
including the tell-tale recollision plateau. Signatures of non-
linear photoemission, though not spectrally resolved, were
found in the initial work on femtosecond laser-driven emis-
sion from nanometer sharp needle tips performed in Stanford
(Hommelhoff et al 2006b, 2006c) and Berlin (Ropers
et al 2007a, 2007c). Based on the previous work discussed
above, it was clear that a strong CEP-dependent current from
metal surfaces, in particular from needle tips, should be
observable, and indeed initial simulations hinted in that
direction (Hommelhoff et al 2006a, 2007, Stockman and
Hewageegana 2007).
We note that (pulsed) electron sources are often
responsible for limiting the maximum achievable beam
brightness in accelerator-related applications. For this reason,
much research has been devoted to pulsed low-emittance
electron sources, but this is outside of the scope of this
review. We refer the reader to the original work based on
needle sources (Boussoukaya et al 1989, Hernandez Garcia
and Brau 2002, Ganter et al 2008). Similarly, in atom probe
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001
tomography, various materials and alloys are cast into needle
form. With either (positive) high-voltage pulses or laser pul-
ses, the tip is decomposed atom by atom. The fragment atoms
are individually analyzed to reconstruct the exact morphology
of the parent material, which is of utmost interest to material
science. Laser-pulse-induced heating of needle tips is there-
fore also investigated in this field (see Miller et al 1996,
Vurpillot et al 2009, Gault et al 2012).
2. Near-field optics at nanotips
Nanometric needle tips give rise to optical near-fields on the
nanoscale, strongly enhancing the electromagnetic field at
sharp geometrical features. Field enhancement plays a key
role in opening up strong-field physics to solid-state systems
for three reasons. First, the requirements on the pulse energy
of the laser source are significantly lowered, so that an
oscillator system with as little as 100 pJ pulse energy is suf-
ficient to observe strong-field photoemission. Second, the
reduced pulse energy and the tiny geometrical cross-section
of the nanotips help to avoid excessive heat deposition and
thermal damage when irradiated with strong laser pulses. By
contrast, strong-field experiments at extended solid surfaces
are challenging due to focal averaging, thermal effects and
space-charge broadening. Third, the optical near-field loca-
lizes photoemission to sub-micron emission areas, enabling
measurements of photocurrents from a single well-defined
emitter. In the following, we will briefly introduce the reader
to the main concepts of near-field optics, before focusing in
depth on nanotips.
2.1. Introduction to near-field optics
For many applications such as microscopy and imaging, it is
of considerable interest to confine the light–matter interaction
to small volumes and length scales. Two length scales are
involved—the optical wavelength and the dimensions of the
object. The first length scale is bound by Abbe’s diffraction
limit of a focused light beam. The second length scale—once
the object’s geometric features are chosen to be much smaller
than the optical wavelength—leads to strong confinement of
the optical field, enabling optics far below the diffraction
limit. Electromagnetic near-fields are induced that are loca-
lized near the object’s surface. Nano-optics, also called near-
field optics, is based on this property and is an active research
field in itself (see, e.g. Maier 2007, Sarid and Challener 2010,
Novotny and Hecht 2012). Nano-optics enables a range of
applications in microscopy and spectroscopy, for example
scanning near-field microscopy (see Wessel (1985), Inouye
and Kawata (1994), Hartschuh (2008)) and tip-enhanced
Raman scattering (see Wessel (1985), Stöckle et al (2000)).
In order to illustrate near-field enhancement, we focus on
the example of a nanosphere as the simplest of all nanometric
geometries. The nanosphere is made of an isotropic material
and is exposed to monochromatic light of wavelength λ in
vacuum. The nanosphere’s radius R is much smaller than λ,
producing sub-wavelength spatial confinement. In linear
4
Topical Review
Figure 1. Nano-optical near-fields at nanostructures. (a) Illustration
of a near-field at a metallic nanosphere induced by a laser field (red).
(b) Normalized local electric field strength at a gold nanosphere,
λ=720 nm.
optics, the electromagnetic response of the material to exter-
nal fields is given by the complex dielectric function
 (l ) =  r (l ) + i i (l ). ò is the square of the complex
refractive index. Assuming a homogeneous static electric field
around the nanosphere, a collective displacement of electric
charge is induced inside the material with respect to the ionic
background. In alternating electric fields, that is, in optical
fields, this displacement starts to oscillate, leading to a time-
dependent polarization (see figure 1(a)). The sphere then acts
as a nano-emitter of light.
For a quantitative description of the near-field, it is
instructive to neglect its time dependence and weak magnetic
field components and make use of the quasi-static approx-
imation (Jackson 1999, Maier 2007). Figure 1(b) shows the
calculated near-field at a gold nanosphere with a radius of
30 nm when applying an optical field with λ=720 nm.
Three main observations can be made. First, at the surface of
the sphere the electric field is strongly enhanced. Second, at
increasing distances from the surface into free space, the
magnitude of the field rapidly decays and eventually returns
to that of the externally applied field. Third, inside the sphere
the local field is homogeneous and its magnitude is much
smaller than that of the applied field—a screening effect.
These three effects, field enhancement, field localization and
screening result from charge redistribution and together form
the pillar of nano-optics.
The maximum local field enhancement ξ, defined as the
magnitude ratio of the total field relative to the applied field,
is found at the poles of the sphere and is given by
 (l ) - 1
x= 1+2 . (1 )
 (l ) + 2
Most significantly, ξ is independent of the radius of the sphere
for spheres that are small compared to λ, but strongly
dependent on the dielectric properties of the material and
wavelength. The enhancement factor for the gold nanosphere
at its optical ‘hotspots’ is ξ=3.41 at 720 nm, corresponding
to a local intensity enhancement of ξ2=11.6. Nonlinear
processes are strongly enhanced at these hotspots, enabling
low-order harmonic generation (Bouhelier et al 2003, Neacsu
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001
et al 2005a, Wolf et al 2016) and strong-field photoemission
(Bormann et al 2010, Schenk et al 2010, Dombi et al 2013,
Keathley et al 2013) for moderately energetic laser pulses or
even continuous wave lasers (Sivis et al 2018).
Nanostructures exist in a large variety of shapes, much
more complicated than spheres. Frequently used examples are
nanotips, nanorods, nanotriangles and composite structures
such as bow-tie antennae and dense nanoarrays. Classical
electrodynamics according to the linear Maxwell equations is,
in most cases, sufficient to understand and simulate the nano-
optical response of such structures. Generally, near-field
formation critically depends on the polarization and wave-
length of the incident light, the geometry of the nanostructure
and on the (wavelength-dependent) dielectric constant of the
material ò(λ). The magnitude of the field enhancement is
related to the absolute value of the complex dielectric func-
tion: the larger ∣ ∣, the larger ξ becomes.
The appearance of nano-optical hotspots is due to the
geometry defining the boundary conditions to Maxwell’s
equations. The external light field induces charges at dis-
continuities at material interfaces and boundaries. If the polar-
ization of the external field is aligned with the normal direction
of sharp features, these charges give rise to strong local fields.
The smaller the length scale of those sharp features such as their
local radius of curvature with respect to the incident wave-
length, the larger the field enhancement becomes. This mech-
anism is the time-dependent analog of the electrostatic
lightning-rod effect and is a common feature for all materials.
A second geometric effect is strongly related to the wave-
length of the light. A linear extension of an odd multiple of half
of the wavelength can cause field enhancement significantly
surpassing the other mechanisms creating an antenna resonance.
Nano-plasmonics adds a third mechanism to near-field
formation, namely localized surface plasmons (LSPs). Refer-
ring to the simple example of the nanosphere, equation (1)
predicts a resonance at òr=−2, a condition called Fröhlich
condition (Bohren and Huffman 1998). The Fröhlich condition
is met by plasmonic metals in the visible spectral region
(òr<0 and 0 <  i  ∣ r∣), such as gold and silver. LSPs can
be excited by direct irradiation or by coupling light through a
grating imprinted on the nanostructure (see, e.g. Ropers
et al 2007b, Berweger et al 2012). Applying the latter method
to a plasmonic nanotip leads to a traveling surface plasmon,
which is focused and ultimately localized at the tip’s apex
(Stockman 2004). With the light on resonance, this naturally
leads to higher field enhancement than other mechanisms
operating in non-plasmonic materials. However, as for every
resonance phenomenon, the build-up of the resonance requires
a characteristic time, which may limit the suitability of such
resonant structures for ultrafast processes.
2.2. Near-fields at nanotips
Nanotips are tapered needles that end in an approximately
conical apex. Usually they are modeled as a hemispherical
apex with radius of curvature R attached to a tapered shank
with half-opening angle θ (see figure 2(a) for an illustration).
The presence of the tip shank introduces a dependence of the
5
Topical Review
field enhancement on both the tip radius and opening angle.
Unlike for nanospheres (see equation (1)) and ellipsoids there
are no analytical formulae available for the field enhancement
at the nanotip geometry. The nanostructure closest to a
nanotip for an analytical solution within the quasi-static
approximation is an ellipsoid (Novotny and Hecht 2012). One
therefore relies on numerical methods to solve Maxwell’s
equations for a realistic incident light field incorporating the
nanotip’s geometrical boundary conditions. Widely used
numerical methods in nano-optics are the finite element
method, the finite-difference time-domain (FDTD) method or
the boundary element method (BEM) (Taflove and Hagness
2005). In the context of strong-field photoemission, both
FDTD and BEM have been successfully applied (see, for
example, the works of Yanagisawa et al (2009, 2010), Thomas
et al (2013, 2015), Förg et al (2016), Ahn et al (2016, 2017)
for FDTD and the study of (Thomas et al 2015) for BEM). In
addition, a discontinuous Galerkin time-domain method has
been developed for nanotips (Swanwick et al 2014). Finite
element methods have been used for simulating static fields
around a nanotip once it is integrated into an electron optical
device (see, e.g. Paarmann et al 2012, Hoffrogge et al 2014,
Bormann et al 2015 McNeur et al 2016, Storeck et al 2017).
Figure 2(a) shows the calculated field strength as a
function of position for a tungsten tip with R=10 nm and
θ=15° and an incident laser pulse with a full width at half
maximum (FWHM) intensity duration of τ=5 fs and central
wavelength λ=800 nm (Thomas et al 2015). The field is
polarized parallel to the tip axis. In this configuration, the
main features of near-field optics, namely field enhancement,
localization and screening of the incident optical field become
apparent. The tip is acting as a highly effective antenna for the
optical field and exhibits strong-field enhancement, with
ξ∼6.5, close to the apex of the tip. Away from the tip
surface, along the symmetry axis, the near-field strongly
decays near-exponentially and relaxes to the field strength of
the incident field. The decay length lF is typically of the order
lF∼0.8 K 0.9R and scales approximately linearly with R.
The value of lF is crucial when describing sub-optical-cycle
electron acceleration driven by the near-field (see Chapter 7).
Inside the tip, screening results in a highly reduced field.
Nanotips for strong-field photoemission can be fabricated
from various conductive materials, such as tungsten, gold,
silver, aluminum or doped silicon (see Chapter 3 for methods
of tip fabrication and characterization). As discussed above, it
is desirable to either choose a dielectric material with a large
absolute value of the dielectric function ò(λ) or to employ an
LSP resonance in a plasmonic material. Figure 2(b) displays
the wavelength-dependent dielectric function of various mate-
rials. For tungsten, gold and aluminum, moving to longer
wavelength in the near-infrared or mid-infrared domain will
increase ∣ ∣ and hence the field enhancement. The increase is
most pronounced for aluminum. Already at 800 nm, the di-
electric function is ò=−64+47i. In addition, gold provides
plasmonic near-field enhancement because its dielectric tra-
jectory in the complex plane (figure 2) passes near òr=−2, the
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001 Topical Review

Figure 2. Near-fields at nanotips. (a) An FDTD calculation solving Maxwell’s equations yields the local electric field strength at the time when the
near-field induced by a 5 fs, 800 nm laser pulse is at its maximum. The nanotip is characterized by the tip radius R and the (half-)opening angle α (here
R=10 nm and θ=15°). The laser field E is linearly polarized along the tip’s pointing direction and travels in the y direction. Gray arrows indicate
the local field direction. (b) Dielectric function for various materials. Real parts òr and imaginary parts òi of the complex dielectric function for tungsten
(W), aluminum (Al), gold (Au) and silicon (Si) as functions of wavelength λ (color). (c) Maximum field enhancement ξ for tungsten and gold nanotips
with varying radius and opening angle (τ=5 fs, λ=800 nm). Adapted from Thomas et al (2015). © IOP Publishing Ltd. CC BY 3.0.

Fröhlich resonance condition for nanospheres (equation (1)).

Note that doped semiconductors such as silicon can also
exhibit strong-field enhancement.
Figure 2(c) shows the geometry dependence of the
maximum field enhancement as a function of R and θ for
tungsten and gold tips irradiated by a typical ultrashort laser
pulse of 5 fs duration and λ=800 nm (Thomas et al 2015).
Three main observations can be made from the numerical
FDTD calculation. First, ξ decreases monotonically with
increasing R for both materials and for any given θ, as
expected. The dependence on R is confirmed by measure-
ments performed on tungsten and gold tips (Thomas
et al 2013, Krüger et al 2014; see figure 3). Second, θ has a
strong influence on the field enhancement, with maxima
around θ=40° and θ=15° for tungsten and gold, respec-
tively. The non-monotonic dependence on θ and the appear-
ance of a maximum at intermediate θ for both dielectric and
plasmonic materials can be traced to the build-up of the
Figure 3. Measured field enhancement factors at tungsten and gold
surface charge density. Its magnitude is controlled by the nanotips. Field enhancement factor of tungsten tips (blue dots) and
interplay between the illuminated surface area increasing with gold tips (red squares) as a function of the tip radius. Uncertainty in ξ
θ and the normal component of the electric field decreasing represents an estimated systematic error due to the uncertainty in
with θ, as predicted by electrostatics. For plasmonic materials, laser intensity. Lines show the results of a numerical calculation of
this effect is further enhanced by the excitation of a surface Maxwell’s equations for 800 nm 5.5 fs laser pulses (W: solid blue
line, Au: dashed red line). Reproduced from Krüger et al (2014).
plasmon, where the resonance condition linking the dielectric © IOP Publishing Ltd. All rights reserved.
constant, wavelength and opening angle leads to a maximum
at smaller angles. This enhancement favors the fabrication of than for tungsten with ξ=12 at θ=35° due to the plas-
tips with small radii and with opening angles near the max- monic response.
imum. Third, the maximum enhancement in the calculated The collective electronic response of the medium leads to
parameter space is ξ=36 at θ=15° for gold, much larger a phase shift Δf between the incident field and the resulting

6
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001
Figure 4. Typical experimental setup for strong-field photoemission
from a metal nanotip. A linearly polarized beam consisting of
femtosecond laser pulses (red) is focused on the apex of a metallic
nanotip with the help of an off-axis parabolic mirror (OAP).
Electrons (blue) are emitted in forward direction and are detected
either using a micro-channel plate (MCP) detector for spatial
resolution or an electron spectrometer for spectral resolution. The
transmitted laser beam can be used for diagnostics.
optical near-field. The magnitude of this retardation effect
also depends on the nanotip geometry and material, but not as
strongly as ξ. For the parameters used in figure 2(c), the
simulations show that tungsten and gold exhibit shifts of
Δf∼0.3 ... 0.6π and Δf∼0.4 ... 0.7π, respectively. Under
pulsed irradiation, the optical response of the nanotip also
leads to small changes in the central wavelength and pulse
duration. In the case of a plasmonic response, long-lived
plasmon oscillations might persist after excitation (see, e.g.
Sönnichsen et al 2002). Nonlinear effects such as second
harmonic generation (Bouhelier et al 2003) can also influence
the optical near-field.
Measuring the strength and shape of near-fields at
nanotips and other nanostructures is possible using a variety
of methods. Nonlinear processes driven by the near-field such
as second harmonic generation (Bouhelier et al 2003, Neacsu
et al 2005a), two-photon photoemission (Tsujino et al 2009),
multiphoton photoemission and strong-field photoemission
(Hommelhoff et al 2006b, Ropers et al 2007c, Grubisic
et al 2013, Park et al 2013, Thomas et al 2013, Krüger
et al 2014, Rácz et al 2017) are extremely sensitive to the
enhancement. Some of the latter investigations also exploit
electron acceleration or recollision driven by the near-field in
order to retrieve the local intensity (for more details, see
Chapter 10). Other methods rely on the interaction of a tightly
focused high-energy electron beam passing by the nanos-
tructure. The near-field manifests itself in triggering cath-
odoluminescence (Vesseur et al 2007, Chaturvedi et al 2009),
incoherent energy loss of the electron beam (Nelayah
et al 2007, Huth et al 2013, Schröder et al 2015b, Yalunin
et al 2016) or coherent electron energy loss and gain (Bar-
wick et al 2009, Feist et al 2015), enabling its spatio-temporal
characterization. Attosecond nanoplasmonic streaking
(Stockman et al 2007, Süßmann and Kling 2011), has been
7
Topical Review
applied to measure the amplitude and phase of a near-field at a
nanotip (Förg et al 2016). Recently, an experiment using
terahertz streaking successfully resolved surface plasmon
propagation at a nanotip (Wimmer et al 2017).
So far, we have discussed optical near-fields within the
scope of classical electrodynamics, which is sufficient for
most applications. However, quantum effects can become
important when considering nanostructures, opening up
‘quantum plasmonics’ (see Zhu et al (2016) for a recent
review). For example, material-vacuum boundaries should
not be considered to be infinitely thin. Instead, the electron
density at the surfaces is smeared out and slightly leaks into
the vacuum (Zuloaga et al 2010). This can lead to an effective
decrease of the magnitude of field enhancement (Zuloaga
et al 2010, Ciracì et al 2012) and can affect plasmonic
antenna resonances in the nano-gap between two nanos-
tructures (Marinica et al 2012, Savage et al 2012, Scholl
et al 2013, Marinica et al 2015). Ab initio theory approaches,
such as time-dependent density functional theory (TDDFT),
are able to provide a self-consistent treatment including such
quantum effects, but suffer from technical limits of current
computing power. An alternative approach introduces
quantum modifications to Maxwell’s equations (Esteban
et al 2012, 2015). To the best of our knowledge, these effects
have not been observed for strong-field-driven nanostructures.
The measurement shown in figure 3 is consistent with the
description by Maxwell’s equations.
Experiments towards and in the strong-field regime were
carried out mostly with nanotips, but there are related
experiments with other types of nanostructures, such as free-
standing nanowire tips with sharp edges (Ahn et al 2017),
nanospheres (Schertz et al 2012), nanorods (Sun et al 2013,
Kusa et al 2015, Lehr et al 2017), nanotriangles (Putnam
et al 2017), nanostars (Sivis et al 2018), carbon nanotubes
(CNTs) (Li et al 2017), composite bow-tie antennas and
nanorod antennas (Dombi et al 2013, Rybka et al 2016,
Hobbs et al 2017, Putnam et al 2017, Rácz et al 2017). In
most of these experiments, the nanostructures were located on
substrates and were made from gold, hence enabling plas-
monic field enhancement when on resonance. In addition,
gas-like ensembles of dielectric nanospheres (Zherebtsov
et al 2011, Süßmann et al 2015, Seiffert et al 2017a, 2017b),
metallic nanoclusters (Passig et al 2017) and C60 ‘buckyballs’
(Li et al 2015) were used in strong-field experiments.
3. Experimental methods
In this chapter, we briefly introduce the experimental methods
that enable strong-field studies at nanotips and other nanos-
tructures. Figure 4 shows a typical experimental setup.
Femtosecond laser pulses are focused onto the apex of a
metallic nanotip situated in an ultrahigh vacuum chamber.
Pressures ideally below 10−8 Pa are helpful to maintain
atomically clean surfaces over at least one hour. The laser
polarization axis is parallel to the tip’s symmetry axis,
enabling maximum field enhancement and pronounced pho-
toemission in the forward direction. Photoelectrons are
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001
usually detected using either a detector with spatial resolution
to image the emission pattern or an electron spectrometer to
measure the photoelectron spectrum. In the following, we will
focus on each element in more detail.
Initial experiments used widely available titanium sap-
phire-based laser sources at a center wavelength around
800 nm generated by both high repetition rate laser oscillator
and low-repetition rate amplifier systems. In oscillator-based
experiments, the damage threshold of the tungsten nanotip
prevented the use of enhanced peak intensities Ieff of more
than 2 ´ 1013 W cm-2 (Krüger et al 2011). Using kHz
repetition rate systems, higher intensities could be reached,
for instance Ieff ~ 5 ´ 1013 W cm-2 for 30 fs, 800 nm pulses
(Bormann et al 2010) and a similar value for 4 fs, 700 nm
pulses (Hoff et al 2017b). Working towards applications of
laser-triggered nanotips as coherent electron guns, blue or UV
laser pulses were employed (see, for example, Ehberger
et al 2015, Bormann et al 2015, Storeck et al 2017). On the
high-frequency frontier, single isolated attosecond XUV
pulses were applied in order to perform attosecond nano-
plasmonic streaking (Förg et al 2016). In the mid-infrared
spectral region, experimental studies relied on fiber lasers
(see, e.g. Thomas et al 2012, Rybka et al 2016, Putnam
et al 2017) or tunable systems based on optical parametric
amplification (see, e.g. Herink et al 2012, Park et al 2012,
Homann et al 2012, Piglosiewicz et al 2014, Förster
et al 2016, Schötz et al 2018). Also, THz pulses were added
to the repertoire of light sources, effectively providing a quasi
DC electric field transient strongly localized at the nanotip
(Herink et al 2014, Wimmer et al 2014, Li and Jones 2016,
Wimmer et al 2017). The laser pulses were delivered onto the
sample most often with reflective optics, such as off-axis
parabolic mirrors or Schwarzschild-type microscope objec-
tives to prevent chromatic aberration and dispersion effects.
Overlapping the nanotip apex with the laser focal spot can be
achieved with the help of 3D nanopositioning translation
stages.
Most experiments are carried out in ultrahigh vacuum,
helping to avoid surface contamination of the sample and
allowing the operation of electron multipliers. An exception
are nano-devices in ambient air where the gap between the
sample and detection electrode is less than 5 μm, sufficient for
electron diffusion to the detector (Rybka et al 2016, Putnam
et al 2017). Nanotips from some materials can be produced
from monocrystalline and polycrystalline wires by electro-
chemical etching, for example, tungsten tips (Klein and
Schwitzgebel 1997) and gold tips (Neacsu et al 2005b, Eisele
et al 2011). Tungsten and to a lesser degree gold enable the
use of field emission microscopy (Fursey 2005) and field ion
microscopy (Müller 1965, Panitz 1982) in order to char-
acterize the field emission properties and the atomic-scale
crystallographic surface structure of the tip apex. Field eva-
poration (Tsong 1990) and resistive flash heating are two
techniques to clean the tip in situ. State-of-the-art nanofabri-
cation techniques such as electron-beam lithography, focused
ion beam milling and epitaxial deposition significantly extend
the range of materials and geometries. For example, recent
8
Topical Review
investigations employed molybdenum nanotip arrays (Mus-
tonen et al 2011), gold nanorod arrays (Dombi et al 2013),
pillar arrays (Nagel et al 2013) and junction devices (Rybka
et al 2016), silver tips (Bionta et al 2016), doped silicon tip
arrays (Swanwick et al 2014), hafnium carbide nanotips
(Kealhofer et al 2012) and carbon cone nanotips (Bionta
et al 2014). In addition, carbon nanotube (CNT) arrays were
used for strong-field experiments (Li et al 2017).
Detection is typically focused either on spatial resolution
or spectral resolution. Spatial information can be gained in a
field emission microscope setup where the nanotip is com-
bined with an MCP detector with a phosphorus screen,
located a few cm away from the tip (see figure 4 and Yana-
gisawa et al (2009) for example experimental setups). The
spatial emission pattern of field emission or photoemission is
mapped on the MCP with a spatial magnification of up to 106,
enabling nanometric resolution without additional electron
optics. Chevron-type MCPs allow detecting emitted electrons
with a typical efficiency of roughly 50%. Spectral resolution
is achieved by electron spectrometers either based on time-of-
flight measurements of laser-triggered electrons (Hilbert
et al 2007, 2009, Keathley et al 2013, Hoff et al 2017b) or on
electrostatic techniques. Typically, retarding field (see, e.g.
Schenk et al 2010, Herink et al 2012) or hemispherical
analyzers (Yanagisawa et al 2011, Park et al 2012, 2013,
Piglosiewicz et al 2014, Yanagisawa et al 2016) are used.
Hemispherical electron analyzers have an additional advan-
tage as they also provide angular resolution. In combination
with an imaging screen around their entrance aperture, they
furthermore allow for site-selective spectral measurements.
Recently, a nanotip has been combined with a velocity map
imaging spectrometer (Bainbridge and Bryan 2014). In order
to use nanotips for electron source applications, they can be
integrated into electron optical imaging systems, both on a
macroscopic (Hoffrogge et al 2014) and microscopic scale
(Lüneburg et al 2013, Bormann et al 2015, Storeck
et al 2017). Typically, a negative bias voltage VDC is applied
between nanotip and detector, leading to a static electric field
of magnitude ∣FDC∣ = ∣VDC∣ (k r r ) at the tip’s apex. The
geometry-dependent field reduction factor kr ranges, typi-
cally, from 5 to 15 for nanotips.
4. Photoemission mechanisms
The near-field induced at nanotips and other nanostructures
opens the door to strong-field photoemission with field
strengths in excess of 1 V Å−1. This is the central theme of
this article, as it enables strong-field physics. In analogy to
gas-phase atomic photoionization, photoemission from
metallic surfaces obeys the intensity-frequency scaling of
Keldysh’s theory (Bunkin and Fedorov 1965, Keldysh 1965).
The dimensionless Keldysh parameter γ is given by
W
g= , (2 )
2Up
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001
where the work function W for the least bound electrons in the
solid replaces the binding energy of the electron in the atom.
The ponderomotive energy Up
e2F02
Up = (3 )
4 mw 2
describes the mean quiver energy of a free electron (electron
mass m and charge e) in a monochromatic light field of
amplitude F0 and angular frequency ω. For the case of a
nanotip, the field strength F0 is replaced by the corresponding
near-field enhanced strength at the tip apex, Feff=ξ·F0.
The Keldysh parameter separates two limiting photoemission
regimes, the multiphoton regime (γ ? 1) and tunneling
regime (γ = 1). In the multiphoton regime, the action of the
light field on the electrons at a metal surface can be treated
within a perturbative approach. In the tunneling regime, this
approach inevitably breaks down since the laser field strength
is starting to compete with the strength of the field binding the
electrons within the metal. In the following, we will survey
important photoemission mechanisms occurring at metal
nanotips and discuss their signatures in experimental data.
4.1. Photoemission assisted by a strong static electric field
In contrast to extended flat metal surfaces (and to nano-
particles in the gas phase), metal nanotips offer the possibility
of also applying a static electric field sufficiently strong for
field emission. At the tip apex, local field strengths of up to
−2 GV m−1 can be easily attained and provide an additional
control knob not available in other geometries. The static field
can also be made slowly time-dependent by applying voltage
pulses (nanosecond time scale, Ganter et al (2008)) or THz
fields (picosecond to femtosecond time scale, see, e.g.
Wimmer et al (2014), Herink et al (2014), Li and Jones
(2016), Wimmer et al (2017)). Before discussing multiphoton
and tunneling photoemission, we will sketch three emission
mechanisms that are enabled by the static field: photoemis-
sion assisted by the Schottky effect, photofield emission and
thermally enhanced field emission.
4.1.1. Photoemission assisted by the Schottky effect. The
photoelectric effect is conceptionally the simplest and most
fundamental photoemission mechanism. Accordingly, the
energy carried by a single photon must be larger than the
work function of the metal, requiring light in the deep UV
spectral region for most materials (Einstein 1905). At metal
nanotips, applying a static electric field leads to a significant
reduction of the potential barrier (see figure 5(a)). This effect
is known as the Schottky effect, here occurring at the metal-
vacuum interface (Schottky 1914). The effective decrease
ΔWs of the work function is given by
∣e∣3 ∣FDC∣
DWs = - . (4 )
4p 0
The Schottky effect enables single-photon (and two-
photon) photoemission at photon energies well below the
work function as ΔWs can reach up to −2 eV. Laser-triggered
9
Topical Review
Figure 5. Emission mechanisms assisted by a static field.
(a) Photoemission assisted by the Schottky effect. The work function
is lowered by ΔWs due to the Schottky effect, enabling
photoemission at photon energies below W. (b) Photofield emission.
After gaining the energy of a photon, an electron is emitted by field
emission. (c) Thermally enhanced field emission. The laser pulse is
heating the conduction-band electrons, resulting in field emission of
excited electrons.
electron gun designs employ this mechanism to localize the
emission to the tip apex (see section 10.2). The static field can
even be used to shape the energy distribution of the emitted
electron pulses by tuning the work function in order to
minimize chromatic electron propagation effects (Hoffrogge
et al 2014, Ehberger et al 2015).
4.1.2. Photofield emission. Photofield emission, also called
photo-assisted field emission, consists of two steps (Lee 1973,
Radoń 1998). First, electrons are excited by single-photon
absorption to unoccupied conduction band states. Second,
field emission induced by the static field leads to emission of
these electrons from the metal surface (see figure 5(b)). The
photofield emission rate depends both linearly on laser
intensity and nonlinearly on the static field strength at the
surface described by the Fowler–Nordheim (FN) theory
(equation (5)). The work function W has then to be replaced
by a reduced barrier height W−ÿω (Lee 1973, Hommelhoff
et al 2006c). The resulting photoelectron spectrum is a
convolution of the laser spectrum with the projected surface
density of states along the laser polarization axis and with the
tunneling probability from the field emission step (Rethfeld
et al 2002). Photofield emission is particularly sensitive to
electronic decoherence effects in the metal. Electron–electron
and electron–phonon scattering inherent to metals and space-
charge effects can strongly influence the electron momentum
spectrum on time scales larger than 10 fs (Rethfeld et al 2002,
Yanagisawa et al 2011, Wendelen et al 2013, Yanagisawa
et al 2016). Photofield emission is not restricted to single-
photon absorption; recently, also two-photon absorption and
subsequent field emission was found at tungsten tips
(Yanagisawa et al 2011, Yanagisawa 2013).
4.1.3. Thermally enhanced field emission. Thermally
enhanced field emission is also a two-step process (Lee
1973, Kealhofer et al 2012) (see figure 5(c)). Compared to
photofield emission, the first step is of a slightly different
nature. Laser light strongly excites electrons within the metal,
creating a non-equilibrium electron distribution. For a
thermalized system of conduction-band electrons, this
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001 Topical Review

corresponds to heating to temperatures of the order of 1,000 K

(Lisowski et al 2004). During and after heating of the electron
gas, electrons transiently occupy states above the Fermi level.
These electrons can undergo field emission if a strong static
electric field is applied to the tip. On the time scales of several
hundred femtoseconds to picoseconds after the excitation,
electron–phonon scattering sets in, leading to a full
thermalization of the metal (Vurpillot et al 2006, Gault
et al 2007). The heating effect depends on many quantities
such as laser average power and peak intensity, pulse duration
and material properties, and competes with all other emission
mechanisms. According to the detailed investigation by
Kealhofer et al (2012), the (electronic) thermal conductivity
is of particular importance. For instance, hafnium carbide,
despite its high melting point and due to its poor electronic
thermal conductivity is much more prone to thermal effects
than metals such as gold and tungsten. Thermally enhanced
field emission has been found to be highly nonlinear in the
laser intensity, more than the usual multiphoton scaling, and
exhibits a strongly localized emission pattern resembling field
emission (Kealhofer et al 2012).

4.2. Multiphoton and above-threshold photoemission

In close analogy to multiphoton ionization in the gas phase,
solid surfaces enable multiphoton photoemission (MPP). Its
main experimental signature is the power-law scaling of the
emission rate w with intensity I0, w µ I0n min , where nmin is the
minimum number of photons required to overcome the work
function. MPP is associated with Keldysh parameters γ ? 1.
Many experimental studies at metal nanotips demonstrated
MPP, for instance Ropers et al (2007a, 2007c), Barwick et al
(2008), Tsujino et al (2008), Hilbert et al (2009) and Yana-
gisawa et al (2011). Only recently, an experiment identified
three-photon MPP by a continuous wave laser field, exploiting
the strong near-field enhancement at metallic nanostar struc-
tures (Sivis et al 2018). MPP is usually mediated by virtual
intermediate states or by resonant states. Resonances allow for
coherent control scenarios, where the spectral amplitude and
phase of a light field controls the spectral amplitude and phase
of an electron wavepacket (see section 10.1).
Moving towards higher intensity and lower γ, substantial
contributions from higher multiphoton orders n>nmin are
expected. More photons than are required to free an electron
are absorbed and ATP takes place, first observed at flat
metallic surfaces (see Luan et al 1989). Detecting ATP
requires spectrally resolved photoelectron measurements
because the photocurrent-intensity power law will be domi-
nated by the lowest multiphoton order. Figure 6(a) displays
the first observation of ATP at a nanotip, recorded at different
incident light intensities (W, λ=800 nm) (Schenk et al
2010). With increasing intensity more ATP peaks appear,
corresponding to the number of absorbed photons. The
spectrum decays exponentially with increasing kinetic energy,
as expected from theory (see Chapter 5). The dependence of
the total photocurrent on intensity shows that three-photon
MPP dominates for all intensities, overshadowing the higher
Figure 6. Strong-field above-threshold photoemission. (a) Count
rate as a function of energy for different incident peak intensities
(W tip, 800 nm). From bottom to top, the intensities are
I0 = {1.9, 2.3, 2.8, 3.2, 3.7, 4.2, 4.6} ´ 1011 W cm-2 . Color sym-
bols mark the features analyzed in (c). Inset: illustration of ATP from
a metal surface. (b) Dependence of the total emission current on
intensity in a double-logarithmic plot. The red line is an MPP power-
law fit to the data, revealing an effective nonlinearity of n≈3.1
(three-photon process). (c) Positions of n=4 and n=5 peaks
(squares and diamonds) and two neighboring minima (circles and
triangles) as function of intensity. The slopes of the linear fit curves
are in the range of −1.2 to -0.2 eV (1012 W cm-2). Adapted figure
with permission from Schenk et al (2010), Copyright (2010) by the
American Physical Society.
orders appearing in the spectral measurements (figure 6(b)).
ATP at nanotips and other nanostructures has been measured
with spectral resolution in many systems and wavelength
regimes, many of them in the strong-field and tunneling
regimes. Prominent examples are Herink et al (2012) (Au tip,
800 nm to 8 μm), Park et al (2012) (Au tip, 1.5 μm), Dombi
et al (2013) (Au nano-array, 800 nm), Swanwick et al (2014)
(n-doped Si tip array, 800 nm), Bionta et al (2014) (W tip,
800 nm), Bionta et al (2016) (Ag tip, 400 and 800 nm),
Förster et al (2016) (W tip, 1.55 μm) and Li et al (2017)
(CNT array, 820 nm). Most of these experiments, however,
do not resolve the ATP peaks; possible reasons include lim-
ited spectral resolution, space-charge broadening and thermal
contributions to the emission, surface impurity of the
employed emitters, a broad distribution of initial states in
energy in the material or intensity averaging due to pulse
envelope effects in the strong-field regime. If photon orders
are not resolved, care must be taken to distinguish the prompt
and coherent ATP from other emission processes.

10
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001 Topical Review

4.3. Onset of strong-field effects

At even higher intensities and lower Keldysh parameters, the

simple picture of MPP and ATP breaks down. Continuum
effects gain importance, in particular the dynamics of the
liberated photoelectron in the laser field, leading to shifts of
ATP peaks and channel closings. The energy of each ATP
multiphoton order reads: Ekin = nw - W - Up  0 . In
analogy to atomic systems (Bucksbaum et al 1987), the peaks
shift towards lower energies and more and more photon
orders will disappear (channel closing). A simple explanation
is provided by the AC Stark effect (or light shift). During the
presence of the laser pulse, the continuum states are field-
dressed and upshifted in energy by the ponderomotive energy
Up (Mulser et al 1993). This energy is lost after the laser pulse
has ended. Strong-field effects are visible in figure 6(a). For
increasing intensity, the peaks shift to lower energy and the
lowest peak (n=3) finally disappears. The shift of the
spectral features is captured quantitatively in figure 6(c).

4.4. Tunneling photoemission

The occurrence of more and more channel closings leads to

strong deviations from the MPP power law. The current-
intensity relation turns into a tunneling rate scaling expo-
nentially with field strength (see equation (7), Chapter 5), a
hallmark of optical tunneling emission. Indications for the
multiphoton-to-tunneling transition at a metal surface were
observed by Tóth et al (1991) and Dombi et al (2010); the
first observation at a nanostructure was reported by Bormann
et al (2010) at a gold tip with a low-repetition-rate amplified
Ti:sapphire laser system. Figure 7(a) shows the main result of
their study: a clearly resolved ‘kink’ in the scaling of the
photocurrent with the pulse energy. A quantitative analysis
reveals a pronounced decrease of the effective nonlinearity
from n∼5 to n∼1 (figure 7(b)); the authors argued that
space-charge saturation can be ruled out since the solid angle
of emission measured with an MCP detector does not increase
with pulse energy. Figure 7(c) shows the result of a calcul-
ation using the strong-field approximation (SFA, see
section 5.3) including field penetration into the metal, clearly
reproducing the transition and elucidating its origin in the
progressive closing of more and more channels.
The transition marked by the ‘kink’ has been observed
and studied in a wide range of systems. Among them are
Keathley et al (2013) and Swanwick et al (2014) (n-doped Si
tip array, 800 nm), Hobbs et al (2014) (Au nano-array,
800 nm), Piglosiewicz et al (2014) (Au tip, 1.65 μm), Kusa
et al (2015) (Au nano-array, 3 ... 10 μm), Rybka et al (2016)
(Au nano-gap device, 1.5 μm), Putnam et al (2017) (Au nano-
array device, 1 μm), Li et al (2017) (CNT, 820 nm) and
Keathley et al (2017) (n-doped Si tip array, 800 nm). In some
studies, including the pioneering work (Bormann et al 2010),
the transition is quite sharp, unlike the predictions of the SFA.
Incorporating the penetration of the laser field into the metal
into the SFA, as suggested by (Bormann et al 2010), can
explain this sharpening; additional processes limiting the
emission rate can be depletion or space-charge effects. The
Figure 7. Transition from the multiphoton to the optical tunneling
regime. (a) Hallmark of the transition is the ‘kink’ in the current-
intensity (pulse energy) scaling (here: Au tip, 830 nm). The slope in
the double-logarithmic plot is changing rapidly from a multiphoton
power-law scaling to a tunneling rate behavior (blue circles:
experimental data; dashed black line: multiphoton power law; red
curve: SFA calculation). Insets: single-shot images of the emission
patterns. (b) Dependence of the effective nonlinearity (red squares)
and solid angle of emission (green circles) on pulse energy.
(c) Results of an SFA calculation including field penetration (total
emission rate: solid black curve; selected individual channels:
colored curves). Increasing the intensity (decreasing γ) leads to the
closing of more and more channels, resulting in the ‘kink’. Adapted
figure with permission from Bormann et al (2010), Copyright (2010)
by the American Physical Society.
observation of a saturation of the intensity dependence of the
current by Piglosiewicz et al (2014) is noteworthy but
remained unexplained. A recent study presented by Keathley
et al (2017) reveals finer structures in the scaling curve related
to single-channel closing, as predicted by the SFA (Yalunin
et al 2011) (see also figure 9 in section 5.3). The authors also
hint at the importance of the initial density of states dis-
tribution for the shape of the transition. Recently, signatures
of the transition have been observed in a very different sys-
tem, a bulk semiconductor nano-device (Paasch-Colberg
et al 2016).

11
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001
5. Theoretical methods
A more detailed understanding of the processes involved in
laser-nanotip interactions requires the development of theor-
etical tools which are discussed in this section. Due to the
design of typical experimental setups (Chapter 3) one is
confronted with a true multi-scale problem: the ground-state
electronic wavefunction typically extends over distances a of
one to a few Ångstroms, the quiver amplitude α of the lib-
erated electron in the enhanced near-field may reach
several nm. The tip radius is about R∼10 nm and the laser
wavelength λ is of the order of 1 μm. Associated time scales
range from a v F ~ 50 as for the electrons in motion (vF K
Fermi velocity) over the laser period Topt∼2.7 fs at a
wavelength of λ=800 nm to the duration of the laser
pulse τ5 fs.
Considering this range of length and time scales, mod-
eling the interaction of laser pulses with metallic nanotips
appears to be a formidable task. However, these widely dis-
parate scales allow for a separation of the problem into a
mesoscopic part for the propagation of the laser pulse in the
presence of the metal tip (solution of Maxwell’s equations;
see above) and a microscopic part for the simulation of the
interaction of the local electric light field with the electronic
system. This is because of the negligible effect of the laser-
induced electron currents (∼1 electron per pulse) on the
propagation of the laser pulse. The solution of Maxwell’s
equations can therefore be directly used as independent input
to any microscopic model for the photoelectron emission.
In the following, we will briefly review the most fre-
quently used methods, which are capable of accounting for
recent experimental observations at least on a qualitative and
often even on a quantitative level. The level of sophistication
ranges from semi-classical approaches including the classical
trajectory Monte Carlo (CTMC) method to solutions of the
time-dependent Schrödinger equation (TDSE) on a single-
particle level to TDDFT as many-body description on a mean-
field level. Representative examples of results from different
methods and comparison with experimental data will be
presented in later chapters. In this chapter, all equations are
given in atomic (Hartree) units (a.u.).
5.1. (Semi-) classical trajectory simulations
In the context of laser-nanotip interactions, (semi-) classical
trajectory calculations closely mirror those employed in laser-
atom interactions, the most prominent of which is the well
known three-step model of high-harmonic generation in laser-
atom interactions. Accordingly, electrons tunnel through the
barrier of the combined surface and laser potentials around
the time of the maxima of the electric field (step 1). The
liberated electrons are then accelerated in free space and
undergo a quiver motion. Depending on the phase of the
driving field at the moment of appearance at the tunneling exit
and the initial momentum, electrons will be either directly
emitted or are driven back towards the surface after an
excursion of about the quiver radius α (step 2). A fraction of
the latter electrons is eventually (back-) scattered at surface
12
Topical Review
atoms and may reach the detector after a second acceleration
cycle in the light field, leading to higher asymptotic kinetic
energies (step 3).
The tunneling step 1 is the key non-classical ingredient
which renders the three-step model semi-classical rather than
classical. Its description can be traced back to the FN theory
for field emission in strong static electric fields (Fowler and
Nordheim 1928, Nordheim 1928). In this seminal work, the
surface potential of the solid was approximated by a potential
step function (deviations of the surface potential from the step
function were considered negligible) of height EF+W, with
EF the Fermi energy of the electron gas and W the work
function of the material. Superimposed with the potential of
the electric field along the surface normal, VDC=FDCz, the
field-dependent current jFN was found to be proportional to
⎡ 4 2 · W3 2⎤
jFN µ FDC
2
exp ⎢ - ⎥, (5 )
⎣ 3∣FDC∣ ⎦
which can be directly converted into a field-dependent
emission rate. A more sophisticated version of the equation
also accounts for the presence of the image-force poten-
tial(see, e.g. Forbes 2006). Applicability of this simple esti-
mate to time-dependent laser fields is far from obvious and is
well justified only in the adiabatic limit. For short tunnel
distances and sufficiently slowly varying fields, the static
approximation provides a good estimate for, now time-
dependent, tunneling rates. Keldysh succeeded in quantifying
‘short’ and ‘sufficiently slowly’ by introducing the parameter
named after him (see equation (2)), which can be alternatively
expressed as
(W ∣F0∣) 2W
g= , (6 )
Topt 4p
relating two time scales, namely the classical time it takes an
electron with velocity 2W to pass through a tunnel of width
W ∣F0∣ with the characteristic time of the oscillating field, i.e.
the optical period Topt. For γ=1 the barrier may be assumed
to be static and equation (5) or a variant thereof can be used.
Typically, this condition is not fulfilled in laser-nanotip
experiments. The use of equation (5) can therefore only be
justified a posteriori when comparing with experimental data.
For example, data from recent experimental studies of pho-
toemission by two-color laser pulses strongly deviates from
predictions based on tunneling rates. Therefore, alternative
emission processes must be involved (Förster et al 2016). For
atomic gases, a closed-form tunneling rate taking the time
variation of the external field into account has been proposed
for nonadiabatic tunneling (Yudin and Ivanov 2001). An
analogous analysis for emission from metal surfaces is still
missing. In most simulations, equation (5) or static emission
rates derived for atoms, e.g. the Perelomov–Popov–Terent’ev
(Perelomov et al 1966), Ammosov–Delone–Krainov (Ammosov
et al 1986) or Delone–Krainov (Delone and Krainov 1994) rates
are used. For laser fields linearly polarized in the direction of
the tip axis and for an electron in the Fermi gas with a
binding energy in the range of W  Wi  W + EF , application
of equation (5) for a ‘slowly’ varying laser field gives rise to a
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001
time-dependent emission rate
⎡ - C2 · W 3 2 ⎤
w (Wi , t ) = f [F (t )] Q [ - F (t )] exp ⎢ i
⎥,
⎣ ∣F (t )∣ ⎦
where f [F (t )] is a field-dependent prefactor to the dominant
exponential and C2 a constant. The Heaviside Θ-function
ensures that, unlike for atoms, emission takes place only during
laser half-cycles with negative field, i.e. when the barrier is
lowered toward the vacuum side. It is important to note that in
this context Ekin = W + EF - Wi is the kinetic energy of a free
electron in the direction of the surface normal. In simple esti-
mates only electrons from the Fermi edge with Wi=W are
considered. For an improved simulation, emission rates w (Wi, t )
are weighted with the projected density of states D (Ekin ) or,
more accurately, the projected surface density of states (SDOS).
The simplest and most popular choice is the SDOS of a free-
electron gas, D (Ekin ) µ(EF - Ekin ).
The tunneling process not only governs the emission rate
equation (7) but also the momentum and spatial distributions,
i.e. the phase-space distribution of the liberated electron. This
distribution provides the initial conditions of the subsequent
classical trajectory calculation. A wide variety of choices of
initial conditions are available.
As for tunneling emission from atoms, position and
momentum distributions at the tunnel exit are a matter of
debate and cannot be reconstructed unambiguously. Estimates
for parallel and perpendicular momentum distributions are
available for atoms (e.g. Delone and Krainov 1994,
Popov 1999), but are missing for metal surfaces. Often, the
simple ansatz for the position at the geometric tunnel exit,
z 0 = W ∣F (t )∣ and p0=0 is used (Krüger et al 2011,
2012a). More sophisticated approaches include corrections of
the position z0 due to the presence of the image potential,
-1 4z , and using a Gaussian momentum distribution for the
emitted electron, thereby approximately accounting for the
position-momentum quantum uncertainty.
In step 2, the electron trajectory can now be easily
simulated numerically by solving Newton’s equation of
motion for a charged particle in the combined fields of the
surface and the external laser pulse,
dVsurf (z)
p = - - F (z , t ) ,
dz
where p is the momentum along the surface normal and F(z, t)
is the effective near-field discussed in Chapter 2.
Depending on the time of emission and their initial
momentum, electrons may escape from the tip region and
reach the detector directly or they may be driven back to the
surface of the solid (indicated in figure 8 by the small light
blue wavepackets). In the former case, a Gaussian momentum
distribution at the tunnel exit will directly result in an expo-
nentially decreasing low-energy spectrum reaching up to
about 2Up (Milošević et al 2006) with a width (1/e-intensity)
directly related to the width of the momentum distribution at
the tunnel exit. Comparison between experimental and
simulated energy spectra in the low-energy region therefore
Topical Review
gives information on the momentum distribution of photo-
electrons upon release from the surface.
(7 ) For a moderate intensity of the IR laser field of
I0 » 5 ´ 1011 W cm-2 at λ=800 nm well below the
damage threshold, the quiver amplitude in the enhanced near-
field, a = x · F0 w 2 » x · 1 a.u. is still small compared to the
characteristic distance over which the near-field enhancement
decays. Therefore, one can simulate the trajectories in a
spatially homogeneous enhanced field ξ·F(t).
An electron emitted at the maximum of the field is
accelerated first towards vacuum for a quarter of an optical
cycle. When the direction of the field reverses it is decelerated
and finally driven back towards the surface which it reaches
close to the end of the next half-cycle with a kinetic energy of
up to 3.17 Up (Milošević et al 2006).
While this is the maximum energy for recombination
and, hence, high-harmonic generation, for electron emission
the third step involves elastic scattering at the surface. For
scattering angles close to Δθ≈π the momentum direction is
impulsively reversed, allowing now for an additional accel-
eration in the complete subsequent half-cycle and leading to
final energies of up to 10.007 Up (second classical cut-off).
The time evolution of the wavefunction of a free electron
in momentum space from emission time t0 to rescattering time
ts is given by Volkov (1935) as
y ( p , ts) = exp [ - iSp (ts, t0)] y ( p , t0) , (9 )
where the Volkov phase is given by the classical action int-
egral,
ts 1
Sp (ts, t0) = òt 0 2
[ p + A (t )]2 dt. (10)
In a semi-classical approximation for the free-particle pro-
pagation, the classical trajectories are endowed with phases
given by the classical actions. Consequently, the Volkov
phase Sp (ts, t0 ) (equation (10)) enters also the semi-classical
description of strong-field dynamics, which allows to selec-
tively incorporate quantum effects (Krüger et al 2011,
2012b). This can be viewed as a partial sum over those paths
contributing to the Feynman path integral that do not involve
classically forbidden trajectories.
(8 ) The quantitative importance of the third step is controlled
by the backscattering cross-section. For the latter, a variety of
approximations are in use ranging from hard-wall scattering
(s  ¥ , p  -p), which is sufficient to reproduce the
plateau and cut-off energy of the photoelectron spectrum
(Krüger et al 2011), to full quantum mechanical doubly
differential elastic scattering probabilities (cross-sections) for
surface atoms modeled by muffin-tin potentials, which also
allow to reproduce the relative heights of direct peak and
plateau (Salvat et al 2005, Wachter et al 2012). In the energy
range considered here, the elastic scattering probability for
electrons with Ekin20 eV off heavy atoms can reach
10%–20%.
Based on the three steps discussed above, the main fea-
tures of the energy spectrum of photoelectrons emitted in
13
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001 Topical Review

Figure 8. Electron dynamics after tunneling. (a) Orange line: laser electric force, blue: direct wavepackets, light blue: rescattered
wavepackets, dashed lines: trajectories suppressed due to screening of the electric field at the surface of the tip. (b) Exponentially decreasing
spectrum due the first direct wavepacket ∣1ñ (blue filled curves). (c) The plateau forms due to rescattering of the wavepacket ∣2ñ (green filled
curves). (d) Repetition of the electron emission after one optical cycle Topt=2π/ω gives rise to interference fringes in the energy spectra
between wavepackets ∣1ñ and ∣3ñ. (e) The full spectrum also includes interferences between rescattered wavepackets ∣2ñ and ∣4ñ and closely
resembles the experimental spectrum (pink). Reproduced from Krüger et al (2012b). © IOP Publishing Ltd and Deutsche Physikalische
Gesellschaft.CC BY-NC-SA 3.0.

ultrashort laser-nanotip interactions can be reproduced: the nanotips (SMMNs), accounting for quantum effects. Con-
exponential drop at low energies and the formation of a sidering that electron emission is confined to the tip apex
plateau with its carrier-envelope phase-dependent cut-off (R∼10 nm), which is much larger than the characteristic
energy (Krüger et al 2011, Wachter et al 2012). In addition, length of the electron wavefunctions (Fermi wavelength
more complex scenarios can be simulated, in particular those λF∼0.1 nm), we find that translational symmetry of the
including the spatial decay of the nano-optical near-field in electron subsystem is approximately conserved in the surface
one or more dimensions. However, the notion of rescattering plane, allowing for a quasi-1D treatment along the surface
breaks down if the quiver length is of the order of the near- normal z.
field decay length or larger (see Herink et al (2012), Park et al For a monochromatic vector potential, A (t ) = -(Feff w )
(2012), Yalunin et al (2013), Piglosiewicz et al (2014), sin (wt ), integral (10) can be solved,
Echternkamp et al (2016b); and Chapters 7 and 8).
⎡ p2
Sp (ts, t0) = ⎢ t + pa cos (wt )
⎣ 2
ts
5.2. Simple man’s model for nanotips Up ⎤
+ Up t - ⎥ , (11)
If interference effects such as the ATP peaks and modulations 2w sin (2wt ) ⎦ t0
in the electron spectrum are also to be included within a
rescattering model, point-like classical electrons have to be and we obtain the wavefunction emitted at time t0 as
replaced by quantum mechanical or semi-classical wave-
y ( p , t , t0) = e-p 4s 2p e-iSp (t , t0 ) eWt0 .
2
packets. Here, we formulate a simple man’s model for (12)

14
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001 Topical Review

Directly emitted electrons will therefore show a momentum 5.3. Strong-field approximation
spectrum of ∣yd ( p )∣2 = e-( p 2) sp or, equivalently, an energy
2 2

The SFA, also called Keldysh–Faisal–Reiss theory (Kel-

spectrum exponentially decaying with decay constant 1 sp2 .
σp can be determined directly from comparison with exper-
imental energy spectra or estimated from theory (Popov
1999).
Those parts of the wavepacket that return to the surface at
time ts are assumed to be elastically rescattered, reversing
their kinetic momentum. After conclusion of the pulse this
part of the initial wavepacket will have a momentum spec-
trum shifted by pr = 2A (ts) - A (t0 ),
∣yr ( p )∣2 = e-[ p - pr ] 2s 2p.
2
(13)
Choosing t0 and ts to maximize pr gives the cut-off energy
pr2 2 » 10 Up . The sum of direct and rescattered momentum
spectra can account for the overall shape of the energy
spectrum quite well (Krüger et al 2012b).
Periodic repetition of emission and rescattering of
wavepackets in subsequent laser cycles at times t j =
t0 + j · Topt and coherently summing up their contributions
results in the emergence of the characteristic ATP peaks in the
energy spectrum. Assuming only two wavepackets launched
at subsequent field maxima (t0=0, t1=Topt) yields the final
momentum spectra for the direct and rescattered parts,
∣yd ( p )∣2 = e-p 2s 2p
2
dysh 1965, Perelomov et al 1966, 1967, Faisal 1973,
Reiss 1980, Gribakin and Kuchiev 1997), successfully
describes photoionization of atoms and negative ions trig-
gered by strong laser fields. It corresponds to a version of a
first-order distorted-wave Born approximation. The distorted
waves used as the final state in the photoionization process
are the Volkov wavefunctions describing free electrons driven
by a light field (see equation (9)), where the atomic potential
is neglected after ionization took place. The SFA to the TDSE
is applicable for calculating electron spectra and ionization
rates for all Keldysh parameters γ, provided that the ioniz-
ation potential is much larger than the photon energy of the
driving-laser field.
The SFA has been first applied to strong-field photo-
emission from surfaces by Bunkin and Fedorov (1965).
Neglecting the projected SDOS, the strongly nonlinear
dependence of the emission rate on the binding energy sug-
gests that the dominant emission processes can be captured by
studying the time evolution of a single active electron at the
Fermi energy, i.e. with a binding energy equal to the work
function of the material. The SFA rate as a function of final
drift momentum p is given by a sum over all channels
corresponding to the absorption of n photons,

⎛ p2 ⎞
´ {cd,1
2
+ cd,2
2
+ 2cd,1cd,2 cos [( p2 2 + Up + W ) Topt ]} w ( p) µ å ∣In ( p )∣2 d ⎜⎝ 2
+ W + Up - nw⎟.
⎠
(16)
n
(14)
Here, we assume a reduction of the problem to one dimension
∣yr ( p )∣2 = e-( p - pr ) 2s p
2 2
and excitation by a quasi-monochromatic laser field. The
theory correctly predicts ATP peaks enforced by the energy
´ {cr,1
2
+ cr,2
2
+ 2cr,1cr,2 cos [( p2 2 + Up + W ) Topt ]},
conservation law in the delta function. The peaks are shifted
(15) to lower energies by the ponderomotive energy Up. The SFA
with ATP maxima at Ekin + Up + W = nw . The large naturally describes channel closing, i.e. due to the ponder-
separation of the two contributions in momentum space omotive action ionization channels are successively sup-
(p0=pr ) allows for a final incoherent summation to obtain pressed as the field strength is increased. Neglecting all spatial
the momentum spectrum, ∣y ( p )∣2 = ∣yd ( p )∣2 + ∣yr ( p )∣2 , dependencies of the transition matrix elements, the coeffi-
which closely resembles experimental spectra. In fact, the cients In(p) are given by
prediction (equations (14), (15)) is sufficiently close to the 2p ⎛ ⎞
1 F
observed spectrum that it can be used to directly determine In ( p ) =
2p ò0 df ⎜ik + p - 0 sin f⎟
⎝ w ⎠
the effective field strength (the free parameter in the model)
present in the experiment. To this end, the static field also ⎧⎡ pF F2 ⎤⎫
´ exp ⎨i ⎢nf + 20 cos f - 0 3 sin (2f) ⎥ ⎬ ,
present should be taken into account. It causes an effective ⎩⎣
⎪
w 8w ⎦⎭ ⎪

decrease of the work function due to the Schottky effect (see (17)
equation (4)). It also leads to a slight decrease of the cut-off with k = 2W (see Yalunin et al 2011). The argument in the
energy, Ecutoff » 10 (Feff - ∣FDC∣)2 4w 2 (Krüger et al 2012b). exponent is related to the action. The integral can be calcu-
Related concepts have been discussed for electron lated numerically. Alternatively, the total emission rate can be
emission from solid surfaces (Yalunin et al 2011, see next obtained to a good degree of approximation using a saddle-
section). In this case, however, the microscopic (electronic point approach. The generalized Keldysh rate, which covers
subsystem) and macroscopic (pulse propagation) models all γ with exponential accuracy (Bunkin and Fedorov 1965,
cannot be separated due to the large extension of the surface. Keldysh 1965, Perelomov et al 1966, Tóth et al 1991) is
Intensity averaging over the beam spot and beam-propagation
⎧ ⎡ ⎤⎫
effects erase irreversibly most of the information about details ⎪ 2 W ⎢⎛ 1 ⎞ 1 + g2 ⎪
⎥ ⎬.
of the photoexcitation process (Lemell et al 2003, Apolonski w µ exp ⎨ - ⎜ 1+ ⎟ arcsinhg -
⎩ w ⎢⎣⎝ 2g 2 ⎠ 2g ⎥⎦ ⎪
⎪
et al 2004), highlighting the importance of studies of photo- ⎭
emission from nanostructures. (18)

15
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001
At large γ, in the multiphoton regime, the total photoemission
rate scales with intensity as a power law, w µ g nmin , where
nmin is the minimum number of photons required to overcome
the binding energy. In turn, the tunneling-like behavior
(see equation (7)) at higher intensities is the consequence of a
rapid sequence of channel closings (see Bormann et al (2010),
Yalunin et al (2011) and figure 7).
Application of the SFA to electron emission from the
metal-vacuum interface requires modifications and extensions
compared to the atomic case due to the broken inversion
symmetry along the surface normal. The laser field is strongly
screened inside the metal and only acts in the vacuum half-
space. Emission only takes place into the positive half-space
away from the surface. Furthermore, inclusion of the rescat-
tering process, which provides a much stronger contribution
for surfaces than for atoms because of the extended nature of
the target, requires a treatment beyond first-order distorted-
wave perturbation theory (Milošević et al 2006). So far, most
investigations have resorted to atom-like semi-classical
models, as described in the previous sections, and only con-
sider electron trajectories on the vacuum side of the interface.
Accurate total photoemission rates, however, require the
inclusion of rescattering at the surface, in particular in the
weak-field regime γ>1.
In a thorough theoretical study by Yalunin et al (2011), a
time-periodic Green’s function approach has been applied to
the problem, providing an approximate solution that includes
the effect of the surface. The key idea is to consider con-
tributions to the total ionization rate due to the reflection of
waves at the surface, with the help of field-dependent
reflection coefficients. This can lead to an increase of the
ionization rate compared to the plain SFA and deviations
from the power-law scaling in the multiphoton regime. The
results of the modified SFA compare well with Floquet
solutions and with a numerical integration of the TDSE (see
figure 9). A different embodiment of the SFA includes the
influence of field penetration into the metal, influencing the
position and shape of the multiphoton-tunneling transition
(Bormann et al 2010).
For a proper description of rescattering photoelectron
spectra, a second-order SFA borrowed from atomic physics
should be applied (see, e.g. Milošević et al (2006) for the
atomic case). Most importantly, the theory predicts inter-
ferences of short and long trajectories, photoelectron yield
beyond the classical rescattering cut-off and a modified
position of the cut-off. In analogy to the HHG cut-off
(Lewenstein et al 1994, Smirnova and Ivanov 2014), the
rescattering cut-off acquires a quantum correction, which
yields an asymptotic value of Ecutoff » 10.007Up + 0.538 W
for γ=1 (Busuladžić et al 2006). Including this correction is
important for precise determination of near-field intensities
from rescattering spectra (Thomas et al 2013, Krüger
et al 2014, Rácz et al 2017, 2018).
5.4. Time-dependent Schrödinger equation
As an alternative to semi-classical or perturbative approaches,
the time-dependent Schrödinger equation can be solved
16
Topical Review
Figure 9. Comparison between different theoretical approaches.
Photoemission rate as a function of Keldysh parameter γ or field
strength (800 nm, W = 5.5 eV): perturbative SFA calculations (solid
orange) are compared to a TDSE solution using the Crank–
Nicholson approach (solid green) and Floquet calculations of the
four-photon (dashed blue) and five-photon (dot-dashed blue)
amplitudes. Adapted figure with permission from Yalunin et al
(2011), Copyright (2011) by the American Physical Society.
numerically,
⎡ 1 ⎤
i¶t y (z , t ) = ⎢ - ¶2z + V (z) + F (t ) z⎥ y (z , t ) , (19)
⎣ 2 ⎦
for sufficiently simple (model) Hamiltonians, in particular on
a single-particle level when many-body effects due to elec-
tron–electron interactions are neglected. The initial state,
ψ(z, t=0), generically the ground state of a single active
electron near the Fermi edge, is propagated according to
equation (19). To recover the main features of the exper-
imental results, the ‘surface’ potential V(z) has to fulfill a few
requirements: the ionization potential in the ground state has
to be equal to W and wavepackets driven back towards the
surface should be reflected with sufficiently large probability.
In its most simple form, square-well potentials are used with
one hard-wall boundary (100% reflection probability). As
refinements, the image-force potential (see, e.g. Hommelhoff
et al 2006b) and the near-field’s spatial decay (Keathley
et al 2017) can be included. To achieve the best agreement
between simulated and experimental peak positions, the depth
and width of the potential well are adjusted to match the
ionization potential and peak positions.
At large distances from the surface the emitted wave-
packet is analyzed by projection onto plane waves of energy
E=k2/2. This can either be done by expanding the wave-
packet into box states ∣fiboxñ with eigenenergy εi, by direct
Fourier transform over the detection region,
dz -ikz
y˜ (k , t ) = ò 2p
e y (z , t ) = y˜ (k ) e-iEt , (20)
where ∣y˜ (k )∣2 is the probability for detection of an electron
with momentum k, or, numerically much more efficient, using
the so-called sampling-point method (Pohl et al 2000). To
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001
obtain the energy spectrum the wavefunction at some detec-
tion point zD is recorded and Fourier-transformed from time to
frequency,
dt iwt
y˜ (zD , w ) = ò 2p
e y (z D , t ).
Outgoing wavepackets, k > 0 can be directly mapped onto
E = k 2 2 = w , yielding the photoelectron spectrum
µ E ∣y˜ (zD, E )∣2 (Dinh et al 2013). The advantage of this
method lies in the much smaller computing box with the
‘detector’ close to the (absorbing) boundary of the system.
A solution of the TDSE for a single active electron in 1D
qualitatively reproduces the ionization rate scaling and the
energy spectrum of photoelectrons with very small numerical
effort. TDSE calculations have been successfully applied to
strong-field photoemission from nanotips and other nanos-
tructures (Hommelhoff et al 2006b, Krüger et al 2011,
Yalunin et al 2011, Krüger et al 2012a, Pant and Ang 2012,
Yalunin et al 2013, Ciappina et al 2014, Zhang and Lau 2016,
Keathley et al 2017). The role of the SDOS in the solid can be
simulated by the incoherent addition of spectra with different
initial energies of the single active electron (Yalunin
et al 2013).
5.5. TDDFT
To reach a higher level of accuracy, the true multi-particle
nature of the electronic target system has to be taken into
account. This can be done by applying DFT (e.g. Parr (1994),
Liebsch (1997) and references therein) for the calculation of
the ground-state electron density of any material. Kohn and
Sham have devised a computationally efficient scheme to
generate the local ground-state density nGS(r) from a sum of
non-interacting pseudo-single-particle wavefunctions (Kohn
and Sham 1965),
n (r ) = å ∣ji (r)∣2 .
i
The orbitals ji(r) are solutions of the single-particle Schrö-
dinger-like Kohn–Sham equation
D
{ -
2
+ Veff [n (r)] } ji (r) = ei ji (r) ,
where the effective potential
Veff [n (r)] = Vion [n (r)] + Ves [n (r)] + Vxc [n (r)]
is a functional of the local density n(r) and includes the
interaction between the electron gas and the ionic cores, the
interaction between electrons, and contributions from
exchange-correlation, respectively. If the correct functional
form of Vxc [n (r)] were known, a self-consistent scheme based
on equations (22) and (23) would converge to the exact
ground-state density nGS(r). In practice, approximations to
Vxc [n (r)] are sought. As an additional simplification the self-
consistency condition for the potential is often abandoned.
Instead, parametrized potentials are used (e.g. Jennings
et al 1988, Chulkov et al 1999), featuring the correct
1 4z -image tail above the surface. To account for rescattering
at the first surface layer(s), a localized potential mimicking
Topical Review
atomic cores can be added, e.g. the screened soft-core Cou-
lomb potential
1
Vatom (z) = e- ∣ z ∣ l TF , (25)
1 + ∣z∣
(21)
with the Thomas–Fermi screening length lTF = EF 3nbulk »
1 a.u.»0.5 Å .
The subsequent time evolution of the system driven by
the external time-dependent potential is described by TDDFT
(Runge and Gross 1984). Similar to ground-state DFT, also
for the time-dependent many-electron system an effective
Schrödinger-like equation for a non-interacting reference
system can be constructed that, if the exact exchange-corre-
lation potential were known, would yield the exact density
and its time derivative of the interacting system (van Leeu-
wen 1999). The time-dependent orbitals ji(r, t) are solutions
of the time-dependent Kohn–Sham equation
i¶t ji (r , t ) = { 1
- [ - i  + A (r , t )]2 + Veff [n (r)]
2 } ji (r , t )
(26)
In practice, suitable approximations to the potential Veff have
to be employed in order to allow for a numerically efficient
solution of equation (26).
Reduction to 1D yields for the density
n occ
n (z , t ) = å ci∣ji (z , t∣2 , (27)
i
with the weighting coefficients ci = ∣Ei - EF∣ p from ana-
lytical integration over the two coordinates perpendicular to
the tip axis and nocc the number of propagated orbitals.
Equation (26) reduces to the 1D Kohn–Sham equation,
i¶t ji (z , t ) = {-¶2z 2 + V [n (z , t )] + Vext (z , t )} ji (z , t ) ,
(28)
(22) with the time-dependent external potential
Vext (z , t ) = z · [FDC + Feff · fenv (t ) · cos (wt + fCE)]. (29)
Here, fenv (t ) is the pulse envelope function, usually of
Gaussian or sin2 shape, and fCE the carrier-envelope phase.
(23) The photoelectron spectrum at the sampling point zD is now
calculated as the weighted sum of equation (21) for all pro-
pagated orbitals,
n occ ¥ 2
(24) P (E ) µ å ci ò-¥ dt eiEt ji (zD , t ) . (30)
i
Using TDDFT detailed comparison between measured
and simulated spectra becomes possible. Figure 10 illustrates,
for the example of a tungsten tip irradiated by a 6.5 fs laser
pulse with λ=800 nm, the potential of such TDDFT (and to
a lesser extent CTMC) methods to successfully simulate and
analyze experimental data.
6. Temporal dynamics of photoemission
In this chapter, we will discuss the temporal dynamics of
strong-field photoemission from nanotips driven by an
17
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001
Figure 10. Comparison between experimental and CEP-averaged
simulated spectra. TDDFT results (solid lines) for different
intensities are compared with an experimental spectrum (symbols)
for I0 = 1.7 ´ 1011 W cm-2 and a classical simulation (green dotted
line), scaled to match the plateau height of the TDDFT result with
identical intensity. Best agreement between experiment and
simulation is obtained for an effective field strength
Ieff = 1013 W cm-2 (field enhancement ξ≈7.5). Adapted figure
with permission from Wachter et al (2012), Copyright (2012) by the
American Physical Society.
ultrashort laser pulse. The basic question posed here is: is the
photoemission prompt, i.e. synchronized with the laser field,
or are there delays of more than, say, an optical cycle
involved? Moreover, according to the simple picture of tun-
neling, we expect bursts of photoelectrons with attosecond
duration to occur at the crests of the driving field, even in the
intermediate regime around γ∼1 (Yudin and Ivanov 2001,
Uiberacker et al 2007). The sub-optical-cycle confinement in
time is appealing since it enables studies of attosecond elec-
tron dynamics at nanostructures. Here, we will discuss
experimental evidence for delayed and prompt photoemission
and present theoretical predictions for the sub-optical-cycle
dynamics.
6.1. Prompt versusdelayed photoemission
Delays in photoemission on the femtosecond and picosecond
time scales are related to an excited electron population per-
sisting even after the pulse has interacted with the sample.
Thermally enhanced field emission is an obvious example,
revealed by measuring arrival times of the electrons at the
detector with respect to the timing of the laser pulse. Clear
evidence of femtosecond delays is provided by experiments in
the multiphoton regime with relatively large tungsten nano-
tips (R∼100 nm) and relatively long laser pulses (∼100 fs)
(Yanagisawa et al 2011, Yanagisawa 2013). Supported by
simulations that include electron–electron and electron–pho-
non scattering, the authors attribute spectral shifts of the
multiphoton peaks to femtosecond delays of the electron
emission with respect to the laser-pulse peak. An extreme
case of multi-electron dynamics is presented by Yanagisawa
18
Topical Review
et al (2016). The authors report signatures of strong space-
charge broadening, distorting the spectral and temporal profile
of the resulting electron bunch with up to 1000 electrons per
pulse at a large tungsten tip. The observation of a pronounced
low-energy peak is associated with the delayed emission of
electrons returning to the tip surface and undergoing inelastic
scattering. Another pathway to uncover delays is measuring
the interferometric autocorrelation trace of the laser pulse
using the nanotip photoemission as a nonlinear element.
Current additivity at long delays indicates prompt photo-
emission and the lack of significant excitation of electrons
participating in the photoemission process, as found for
sharper tips and shorter laser pulses (Hommelhoff
et al 2006b).
A systematic investigation of delays in the multiphoton
regime is presented by Juffmann et al (2015). Photoelectrons
produced from a tungsten tip (R∼400 nm) by 10 fs, 800 nm
pulses were streaked in a microwave cavity, mapping their
emission time onto energy shifts of the photoelectrons with
2 fs accuracy. The investigation was carried out for Keldysh
parameters 19.1>γ>6.6 (using the incident field strength
in equation (6)). Below γ∼13 the data is clearly compatible
with prompt emission (figure 11). The authors speculate that
the measured delays could represent Keldysh tunneling times.
6.2. Sub-optical-cycle photoemission dynamics
Ab initio theory provides direct insight into the attosecond
dynamics of strong-field photoemission, without the need to
rely on drastic approximations. A TDSE calculation shows
that the temporal profile of the surface current changes sig-
nificantly around γ∼1. It switches from following the light
field’s vector potential, accompanied by very little net emis-
sion current, to following the positive crests of the laser field
itself, indicating the emergence of the tunneling regime
(Yalunin et al 2011). The sub-cycle resolving tunneling pic-
ture appears to remain valid even around γ∼1, as revealed
by TDSE calculations (Hommelhoff et al 2006b, Krüger
et al 2012a). TDDFT (section 5.5) provides insight into
temporal dynamics including multi-electron effects, in good
agreement with experimental results (see figure 10). As an
example, we discuss the result for a tungsten tip irradiated by
an 800 nm laser pulse with τ=6.5 fs and an effective max-
imum field amplitude of Feff=0.02 a.u. (Ieff = 1.4 ´
1013 W cm-2 , γ∼2). In this example, the static bias field is
chosen to be two orders of magnitude smaller (figure 12(b)).
Inside the tip (z„0), the external laser field induces
density fluctuations (surface polarization) close to the surface
screening the external field in the interior. The time scale of
the variation of the driving field (T≈110 a.u. ≈ 2.7 fs) is
slow compared to the time scale of the electronic subsystem
of the tip given by λF/vF≈5 a.u. ≈ 125 as suggesting an
almost adiabatic adjustment of the electron gas to the external
optical field. This is confirmed by the electric dipole moment
(panel (b)), which is almost perfectly in phase with the
driving field. The density change induced at the surface is less
than 1% of the total density in the electron gas (figure 12(a)).
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001
Figure 11. Emission time delay in the multiphoton regime (axis on
rhs) and microwave-induced energy shift (axis on lhs) as a function
of intensity. Delays are only observed below 75 GW cm−2 (γ∼13).
A fit curve (blue) displays the emission time delay Δt derived from
Keldysh theory. Adapted figure with permission from Juffmann et al
(2015), Copyright (2015) by the American Physical Society.
Figure 12. TDDFT simulation of electron emission and rescattering. (a)
Absolute value of the induced density dn (z, t ) = ∣n (z, t ) - n GS (z )∣.
Full vertical arrows mark maxima of the electric force. Dashed lines
follow trajectories of rescattered electrons. Interferences in position
space with increasing slopes (velocities) are the signature of the equi-
spaced multiphoton peaks in the electron energy spectra. (b) Full red
line: laser electric force Feff(t); dashed purple line: time-dependent
dipole moment (arb.u.); dash-dotted green line: static field FDC.
Reproduced with permission from Wachter (2014).
Turning to the vacuum side (z>0), we find the physical
picture developed in Chapter 5 confirmed. Electron emission
is concentrated around the maxima of the external field
indicated by vertical arrows. Electrons are then accelerated
towards the vacuum (subsequent half-cycle), turn around at
the opposite field maximum and are driven back to the surface
from where a fraction of the impinging wavepacket is
rescattered (classical trajectories indicated by dotted lines).
Rescattering will be the focus of the next chapter. As the
emission sequence is repeated for every laser cycle, emitted
19
Topical Review
wavepackets interfere, leading to ATP peaks in the energy
spectrum of emitted electrons separated by ÿω. The slope of
the maxima of δn(z, t) (figure 12(a)) indicates the velocity of
outgoing electrons. Classically, the largest slope would cor-
respond to a kinetic energy of 10 Upindicated by the dotted
arrows for rescattered electrons reached for a pulse with
suitably chosen CEP (minus-cosine-pulse). Indeed, structures
with similar slopes are reproduced by TDDFT, identifying the
rescattering mechanism as the origin of the high-energy pla-
teau in the energy spectra.
7. Acceleration and recollision of photoelectrons
In this chapter, we discuss electron dynamics after photo-
emission as the electrons are driven and accelerated by the
strong laser field. Electrons start to quiver in the laser field,
with a quiver amplitude of a = ∣e∣Feff (mw 2 ). At nanotips,
and in contrast to gas-phase photoionization, a second length
scale, the near-field decay constant lF, plays an important role.
As discussed in Chapter 2, lF is of the order of the tip radius
R. As the electron starts moving away from the surface, it may
experience the decay of the near-field. A spatial adiabaticity
parameter δ can be defined when comparing the two length
scales (Herink et al 2012),
lF l mw 2
d= = F . (31)
a ∣e∣Feff
For d  1, the electron experiences an approximately con-
stant laser field during one laser cycle. This enables the
observation of recollision phenomena, closely mirroring
recollision in the gas phase. This picture changes once we
cross into δ<1 where the dynamics are strongly modified.
Here, the electrons ‘surf’ down the near-field even before they
are able to perform significant quiver motion opening up a
true sub-optical-cycle regime of photoemission and accel-
eration (Herink et al 2012). The research performed with
nanostructures, as presented here, is closely related to surface
plasmon-driven acceleration at metal surfaces (see, e.g. Irvine
et al (2004), Dombi et al (2010), Rácz et al (2011), Földi et al
(2015) and the theoretical study of Rácz and Dombi (2011),
who predicted effects of non-quiver electron acceleration).
This chapter is divided into two sections, discussing rescat-
tering effects (δ>1) and sub-optical-cycle accelera-
tion (δ<1).
7.1. Electron recollision and rescattering at nanotips
The first observation of recollision and rescattering at a metal
surface was reported by Krüger et al (2011) followed by more
systematic investigations by Wachter et al (2012) and Krüger
et al (2012b). Figure 13(a) shows an intensity scan of ATP
spectra recorded at a tungsten tip. With increasing laser
intensity, a plateau develops in the high-energy region of the
spectrum with the count rate barely changing as a function of
energy. The plateau is terminated by a cut-off, which depends
linearly on intensity, as predicted by the 10 Up law. The
generation of the plateau is tied to the three steps of the
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001 Topical Review

Figure 13. Rescattering plateau in above-threshold photoemission. (a) Intensity scaling of the rescattering plateau. From bottom to top, the
incident intensity is I0 = {0.55, 0.72, 0.89, 1.1, 1.3} ´ 1011 W cm−2 (W tip, 800 nm, 6 fs). The exponential decay (direct electrons) is
followed by a plateau (rescattered electrons). The crossing points of the linear fit curves indicate the rescattering cut-off position. Inset: cut-
off energy as a function of intensity (red line: linear fit). Reproduced from Krüger et al (2012b). © IOP Publishing Ltd and Deutsche
Physikalische Gesellschaft. CC BY-NC-SA 3.0. (b) Comparison of experimental data (Krüger et al (2011), green dots) with TDSE
calculations (Yalunin et al (2013), solid green curve). For comparison, we also show results with only a single initial state (solid black curve)
and with rescattering switched off (dashed black curve). Yalunin et al (2013) © 2013 by WILEY‐VCH Verlag GmbH & Co. KGaA,
Weinheim. (c) Plateau in strong-field photoemission from Au nanorod and bow-tie arrays (800 nm). Three classes of nanorod geometries
were used, resonant (gray), red-detuned (red) and blue-detuned (blue) with respect to the laser wavelength of 805 nm. At identical incident
intensity (I0 = 2.5 ´ 1010 W cm−2), different geometries lead to variations in field enhancement, causing differences in the achieved cut-off
energy. Reprinted (adapted) with permission from Dombi et al (2013). Copyright (2013) American Chemical Society. (d) Low-intensity
(blue) and high-intensity (green) photoelectron spectra from a Si nanotip array. Reprinted (adapted) with permission from Swanwick et al
(2014). Copyright (2014) American Chemical Society. Further permissions related to the material excerpted should be directed to the ACS.

recollision picture: sub-cycle-resolved tunneling, acceleration
by the laser field and finally elastic scattering, the shape of the
plateau is a result of their interplay. Although recollision does
not necessarily need to feed on the tunneling photoemission
mechanism since it is mainly a result of field-driven dynamics
(steps 2 and 3), the shape of the plateau indicates that a sub-
optical-cycle tunneling rate with a maximum around the peak
of the laser field is responsible for the emission step. Tun-
neling also causes a slight displacement of the photoelectron
from the surface when it appears in the continuum, leading to
a modified cut-off law Ecutoff » 10.007 Up + 0.538 W .
Clear signatures of rescattering at δ?1 have also been
observed at Au nanoarrays (Dombi et al 2013, Kusa et al 2015,
Rácz et al 2017), see figure 13(c), n-doped Si nanotip arrays
(Swanwick et al 2014), see figure 13(d), and Ag nanotips (Bionta
et al 2016). The pronounced dependence of rescattering on the
sub-optical-cycle waveform of the driving field is the subject of
the next chapter. Krüger et al (2012b) explored the effects of an
additional static electric field, which pushes the cut-off towards
slightly lower values, in agreement with TDDFT calculations.
TDDFT (Wachter et al (2012), Krüger et al (2012b); see
figure 10), TDSE (Krüger et al 2011, 2012a, Yalunin et al 2013),
(semi-)classical trajectory calculations (Krüger et al 2011, 2012a,
Wachter et al 2012, Dombi et al 2013, Rácz et al 2017, 2018)
and the SMMN (Krüger et al (2012b); see figure 8) are able to
reproduce the experimental data even to a quantitative degree;
figure 13(b) shows a TDSE calculation with excellent agreement
with the experiment (Yalunin et al 2013). The ATP peaks are
smeared out, mostly due to the superposition of a broad dis-
tribution of initial states. In the TDSE the backscattering can be
switched off, leading to the disappearance of the plateau.
7.2. Sub-optical-cycle electron acceleration in near-fields
In order to decrease δ (equation (31)), it is convenient to move
to longer wavelengths than the often used 800 nm driving

20
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001
Figure 14. Sub-optical-cycle acceleration regime. (a), (b) Photo-
electron trajectories driven by ultrashort pulses depend strongly on
whether the quiver amplitude is (a) smaller (δ ? 1, short-wavelength
irradiation) or (b) larger (δ = 1, long-wavelength irradiation) than
the decay length of the nano-optical near-field (white region). In (b),
the electron escapes the near-field before substantial acceleration
back to the surface. (c) Energy spectra as a function of wavelength
for approximately constant intensity (Au tip, R = 12 nm). At long
wavelengths, the cut-off of the spectrum is wavelength-independent
and solely determined by the intensity—hallmarks of sub-optical-
cycle acceleration. (d) Cut-off energy (circles, upper panel) as a
function of wavelength for two values of total emitted charge. The
curves represent upper and lower bounds to the cut-off as calculated
with classical trajectory simulations including the near-field decay,
corresponding to local intensities of I1 = 5.4 TW cm-2 (dashed) and
I2 = 40 TW cm-2 (solid). Dash-dotted curve shows the theoretical
cut-off when neglecting the near-field (I2). (e) Spatial adiabaticity
parameters δ as a function of wavelength. Adapted by permission
from [Springer Nature]: [Nature] (Herink et al 2012), Nature 483
(7388), 190.
field (see figures 14(a), (b) for an illustration). The first
observation of sub-optical-cycle acceleration in a nanotip
near-field was presented by Herink et al (2012), carried out at
sharp Au tips with a wavelength-tunable laser system.
Keeping the peak field strength Feff approximately constant,
they used short pulses at five different center wavelengths
ranging from 800 nm–8 μm and measured electron spectra
(see figure 14(c)). At long wavelength, as we cross into
δ<1, the cut-off kinetic energy deviates strongly from the
10 Up-law and becomes independent of wavelength. Virtually
no quiver motion takes place and the acceleration occurs
within less than an optical cycle (see figures 14(d) and (e)).
Solely the peak field strength Feff governs the acceleration
and determines the shape of the spectrum.
The effect has been further investigated in a systematic
study (Echternkamp et al 2016b) and is also applicable to
different systems such as CNTs where the near-field decay
21
Topical Review
length can be extremely small (Li et al 2017). The initial
observations have been supplemented by spectral measure-
ments with angular resolution, exploring the vectorial nature
of the near-field gradient (Park et al 2012, 2013). The sub-
optical-cycle acceleration leads to an energy distribution with
a narrower cone opening angle than the recollision mech-
anism. A recent study focused on a low-energy peak at δ∼1,
reporting an intensity-dependent shift due to a nonadiabatic
ponderomotive shift (Schötz et al 2018). Sub-cycle accel-
eration is intrinsic to THz-driven electron emission from
nanotips (Herink et al 2014). Kinetic energies of up to 5 keV
have been reported (Li and Jones 2016), opening up appli-
cations as a source of high-energy electron pulses.
8. Sub-optical-cycle waveform control of electron
dynamics
Since tunneling photoemission and electron acceleration from
nanotips are driven by the sub-optical-cycle waveform, these
mechanisms can be controlled by shaping the laser field. To
this end, delicate control over the temporal electric field of the
laser pulses is required. Two options are frequently used: the
use of ultrashort few-cycle pulses with control over their CEP
fCE and the use of (longer) two-color pulses with control over
the relative phase of the two colors. Either method exploits
the exponential sensitivity of the emission probability on the
field amplitude in combination with symmetry breaking at the
metal surface. In this section, we will discuss the first option,
the influence of the carrier-envelope phase of ultrashort laser
pulses on the regimes δ>1 (rescattering) and δ<1 (sub-
optical-cycle acceleration). To the best of our knowledge,
two-color pulses have only been applied in the multiphoton
regime (see section 10.1 for more details).
8.1. Waveform control of rescattering
As discussed earlier (section 5.2), the cut-off energy of the
plateau depends on the kinetic energy of the electron wave-
packet upon rescattering from the tip surface. Maximum
kinetic energy requires maximum force driving the electron
back to the surface, i.e. a strong dependence on fCE is
expected. On top of these classical dynamics of the laser-
driven electron, the CEP is affecting the field-cycle-resolved
tunneling probability. Figure 15 shows the results of a CEP-
resolved strong-field experiment with ∼6 fs pulses at 800 nm
at Keldysh parameter γ≈2 (Krüger et al 2011). An FWHM
intensity pulse duration of 6 fs translates into ∼2.5 optical
cycles, enabling pronounced CEP effects. The count rate is
found to be strongly modulated by fCE over the whole
spectral range, as evidenced by modulation depths ranging
from a few percent in the direct part up to 100% above the
cut-off (figure 15(a)).
Upon closer look, two distinct phase-dependent effects
are found in the CEP-resolved data (figure 15(b)). First, the
variation of the cut-off position with CEP is solely related to
the field-driven dynamics of the liberated electron. The
waveform defines the field that the electron experiences
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001
Figure 15. Waveform-controlled rescattering. (a) CEP-averaged
photoelectron spectrum (blue solid curve) consisting of the direct
part (Ekin  4 eV) and the rescattering plateau. Green points show
the modulation depth of the count rate variation when scanning the
CEP. (b) Color plot showing CEP-resolved spectra on normalized
linear color scales, defined separately for the direct and rescattered
parts. Data have been recorded over a range of 2π and extended to
4π for better visibility. Yellow circles indicate the positions of the
cut-offs (red solid curve: sinusoidal fit). (c) Contrast of four spectral
peaks in the plateau as a function of the CEP (blue diamonds; red
solid curve: sinusoidal fit curve). Adapted by permission from
[Springer Nature]: [Nature] (Krüger et al 2011) Nature 475
(7354), 78.
between photoemission and rescattering, determining the
amount of acceleration up to the time of rescattering and then
towards the detector. The second effect reflects quantum
interference: the contrast of the peaks in the plateau depends
strongly on the CEP ranging from below 10% (fCE ~ 0 ) to
30% (fCE∼π, see figure 15(c)). In a simplified one-electron
picture, the high-contrast case corresponds to a scenario
where two subsequent cycles lead to the generation of elec-
tron wavepackets that end up at kinetic energies in the pla-
teau. Their interference leads to spectral fringes, adding a
temporal perspective to the notion of ATP peaks. In the low-
contrast case, only a single optical cycle within the pulse
contributes a rescattered wavepacket. Therefore, no fringes
are expected. In essence, we find here a transition from a
temporal double- to a single-slit scenario, fully controlled by
the waveform of the driver pulse. Such scenarios have also
been found in atomic strong-field photoionization (Lindner
et al 2005), cold atom optics (Szriftgiser et al 1996) and
neutron interferometry (Hils et al 1998). The spectral fringe
spacing is related to the temporal separation of the emission
of the wavepackets through a Fourier relation, ΔE=h /Δt.
Assuming Δt to be equal to the optical-cycle duration (2.7 fs),
we end up with the photon energy (1.55 eV). Accordingly, the
observed tilt of the fringes (see figure 15(b)) reflects a varying
temporal separation, as confirmed by a Fourier analysis of the
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Topical Review
Figure 16. Carrier-envelope phase dependence of photoelectron
spectra. (a), (b) Experimental data (Krüger et al 2011) shown as
normalized asymmetry signal (equation (32)). Increased signal (large
cut-off energy) is shown in blue, reduced emission in red. (a) Raw
data, (b) smoothed over 1.5 eV and 0.5 π. Absolute phase has been
adjusted to match results of the TDDFT simulation (c), (d). (c) raw
data, (d) smoothing as for experiment. (e) CEP-dependent spectrum
modeled by the SMMN. Figure from Wachter (2014).
CEP-dependent spectra (Ott et al 2013). The spectral width of
the plateau (9 eV) gives a rough estimate of the duration of
the temporal slit (450 as) through Heisenberg’s time-energy
uncertainty relation.
The experimental data have been successfully modeled
with a semi-classical three-step model including quantum
interference and a TDSE calculation (Krüger et al 2011,
2012a). Comparing TDDFT results to the fCE-resolved
experimental data (figure 16) provides a stringent test of the
accuracy of the simulation and reveals excellent agreement
between theory and experiment over the full spectral range,
including the position of the ATP peaks and even some of the
fine structure. Figure 16 displays this asymmetry A of the
normalized electron spectra as a function of fCE. The asym-
metry is given by the electron spectrum divided by the CEP
average over all spectra,
P (E , fCE)
A= . (32)
ò dfCE P (E , fCE)
The dominant feature in the data is a large-scale structure of
bent stripes that converge towards a maximum at fCE=π
(minus-cosine-pulse) for large electron energies. Such bent
stripes have also been observed in electron spectra from
atoms (Paulus et al 2003, Milošević et al 2006) and dielectric
nanospheres (Zherebtsov et al 2011, 2012) and have been
exploited to determine the CEP in single-shot measurements
(Wittmann et al 2009, Johnson et al 2011, Rathje et al 2012).
A simple estimate (Chapter 5) provides an intuitive
understanding of the CEP dependence of photoemission.
Assuming electron emission at the field maximum t0, the shift
of the rescattered momentum distribution pr in equation (13)
reduces to pr = 2A (ts) with ts determined by the solution of
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001
Newton’s equations for an initial momentum at the tunnel exit
of p(t0)=0 (section 5.1). Obviously, the resulting trajectories
and rescattering times ts are sensitive to the CEP leading to
the observed CEP-dependent shift of the high-energy part of
the electron spectra. More elaborate calculations using the
SMMN (section 5.2) lead to the asymmetry structure shown
in figure 16(e), closely resembling the experimental and
TDDFT results. Both the bent-stripe structure including the
curvature and the slope of the low-energy part resulting from
the interplay of the strongly nonlinear tunneling rate and the
rescattering process are reproduced. For fCE=π (minus-
cosine-pulse), rescattering is strongest, leading to the largest
cut-off energy and largest number of electrons at high ener-
gies (blue). The tunneling probability at the maximum pre-
ceding the minus-cosine peak is, however, smaller than, e.g.
for a plus-sine-pulse, for which, in turn, a smaller rescattering
energy is found. Overall, this interplay underlies the bent-
stripe pattern in the CEP dependence.
The near-perfect agreement between model calculations
and experimental data in combination with simulations of
pulse propagation (phase shift of the near-field at the surface
induced by the nanostructure) opens up the possibility to
determine the absolute phase of ultrashort laser pulses by
recording photoelectron spectra in laser-nanotip interactions
(see section 10.1).
8.2. Waveform control of sub-optical-cycle acceleration
Kinematic CEP effects in the tunneling regime g  1 and
sub-optical-cycle acceleration regime have been investigated
by Piglosiewicz et al (2014). The authors used CEP-stable
16 fs 1.65 μm pulses in order to drive strong-field photo-
emission from a gold nanotip, with an enhanced field strength
of Feff » 15 V nm-1. Figure 17(a) shows CEP-dependent
spectra. Both the low-energy and the high-energy cut-offs of
the spectrum depend on the CEP; their positions oscillate
approximately out-of-phase (figure 17(b)). Classical trajectory
calculations, taking into account a very small near-field decay
constant, match the experimental results (figures 17(c), (d)).
The waveform predominantly affects the dynamics of the
accelerated electrons.
Another route to explore the temporal dynamics in the
sub-optical-cycle acceleration regime has been implemented
by Echternkamp et al (2016b). At the long-wavelength
frontier, the authors employed ultrashort laser pulses at
8.7 μm. Then, only one optical cycle contributes to the
emission; a single wavepacket is generated and immediately
accelerated in the near-field without any further interaction
with the surface. With the knowledge of the dynamics of the
electron inside the near-field, the spectral shape of the emitted
photoelectrons can be directly mapped on the sub-optical-
cycle emission rate (see figure 18). The reconstructed rate
agrees well with the FN tunneling rate (equation (5)), con-
firming its suitability to describe tunneling photoemission
from metallic surfaces.
23
Topical Review
Figure 17. Waveform control of sub-optical-cycle acceleration.
(a) CEP-resolved energy spectra (Au tip, 1.65μm). Clear modulation
of both low-energy and high-energy cut-offs are observed, marked
by red and black circles, respectively. (b) Position of low-energy cut-
off (red triangles) and its high-energy counterpart (black circles) as a
function of the CEP. Solid curves represent sinusoidal fits; the two
cut-off energies oscillate almost fully out-of-phase. (c), (d) Classical
trajectory calculation results for both cut-offs. Adapted by permis-
sion from [Springer Nature]: [Nature Photonics] (Piglosiewicz
et al 2014), Nat. Phot. 8, 37.
9. Harmonic generation
So far, we have focused on the energy spectra of the electrons
photoemitted from a metal nanotip by ultrashort laser pulses.
In this section, we will discuss another consequence of
strong-field laser-matter interaction, namely the emission of
radiation with photon energies of n·ÿω, a process known as
HHG. HHG from atoms is well understood based on the
three-step model. Although not experimentally demonstrated,
the possibility of plasmon-enhanced gas-phase HHG has
triggered extensive theoretical work (see, e.g. Yavuz et al
(2012), Ciappina et al (2012), Lupetti et al (2013), Pérez-
Hernández et al (2013), Wang et al (2017), Yuan et al (2018),
for the influence of plasmonic effects on field enhancement
for nanotips see Chapter 2). Three-step models of HHG from
bulk solids in momentum space have only recently been
proposed (see, e.g. Golde et al 2008, Vampa et al 2014,
Higuchi et al 2014, Vampa and Brabec 2017, Chizhova et al
2017). For atoms, a high-energy cut-off at Ecutoff = Ip +
3.17 Up was predicted from classical trajectory analysis and
confirmed in experiment. For solids and surfaces of nanos-
tructures, the influence of collective effects, e.g. plasmon
excitation, on HHG is difficult to assess. A single active
electron TDSE calculation has been performed to study HHG
from nanotips (Ciappina et al 2014). Here, we will use
TDDFT to investigate HHG from nanotips and provide esti-
mates for the possibility to observe the emission of high-
energy photons in experiment.
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001 Topical Review

Figure 18. Reconstruction of the sub-optical-cycle emission rate. (a) Time-to-energy mapping (blue) enables the reconstruction of the
instantaneous rate from the electron spectrum ((b), driven by a 8.7 μm pulse). The reconstructed rate compares well with the FN rate (gray).
Adapted by permission from [Springer Nature]: [Applied Physics B: Lasers and Optics] (Echternkamp et al 2016b), Appl. Phys. B 122
(4), 80.

To the best of our knowledge, direct HHG from nanos-

tructures including metal tips has not been observed. The
reason for this can be found by an order-of-magnitude esti-
mate for the emission rate of HHG from a nanostructure
compared to that for HHG from a gas of atoms. The number
of gas atoms in the laser focus is typically about 1010, while
the surface of a nanotip of radius 10 nm only contains about
5000 atoms. This huge disparity in the number of potential
emitters considerably reduces the emission rate and, thus, the
likelihood for the observation of HHG from isolated nanos-
tructures. We can further estimate the order of magnitude of
the linear response at the driving frequency. Modeling the
Figure 19. Simulated HHG spectra from metallic nanotips.
metallic nanotip as a nanosphere of the same radius R as the
(a) Harmonic spectra for Feff=0.005, 0.01 and 0.018 a.u. The
tip, the induced dipole moment, dielectric response of the system to a δ-kick containing all
e-1 frequencies is shown in red. (b) Time-frequency analysis of emitted
d (w ) = R F0 » R F0, e  1, (33) radiation for Feff=0.018 a.u. The highest harmonics well above the
e+2 cut-off energy of HHG in atoms are emitted in time close to the zero-
crossings of the driving-laser field (c) when emitted electrons are
at the driving wavelength in linear response serves as a
rescattered at the surface (vertical dotted lines). Figure from
measure of its scattering power. The angle-integrated emitted Wachter (2014).
radiation calculated from the dipole acceleration is then given
by (Jackson (1999))
dotted lines in panel (b)). Note that in this (nearly) free-
4p ⎛⎜ 2p ⎞⎟4 6 e-1 2

ò dW∣Escat∣2 = F02
3 ⎝l ⎠
R
e+2
. (34)
For typical ultrashort pulses employed in laser-nanotip
interactions (I0 = 1.1 ´ 1011 W cm-2 , focus size ∼1.5 μm,
τ=6.5 fs, λ=800 nm), only about half a photon is scattered
on average for the incident number of photons, in our
example more than 108. This sets the scale for the results
shown in figure 19. The total spectrum (∣d̈ (w )∣2 shown for
various intensities) features a strong linear-response peak at
ÿω, three orders of magnitude more intense than the plateau
region extending up to the plasmon energy. High-energy
components of the spectrum are observed up to around
W + 3.17Up + wp (panel (a)), with ωp the plasma frequency
and Up calculated from the locally enhanced field strength
Feff. The appearance of even harmonics is a consequence of
the broken symmetry at the surface. Time-frequency analysis
of the emission process, i.e. a windowed Fourier transform,
relates the emission times of the most intense harmonics with
the recollision times of the photoemitted electrons (vertical
electron gas calculation the influence of the plasmon excita-
tion, in particular the extension of the plateau region by the
plasmon energy ÿωp, is clearly visible and differs from atomic
spectra. This extension can serve as an indicator for possible
metal-surface and nanostructure effects.
Comparison of our estimate for the linear response with
the intensity of higher-order harmonics in figure 19 gives an
impression of the expected photon yield. Taking for example
the 7th harmonic around 11 eV photon energy and taking the
reduction of the intensity of the plateau compared to the
response at the driving frequency, we arrive at a yield of
∼10−3 harmonic photons per laser pulse. This small signal
can only be mitigated by an increased repetition rate of the
incident pulsed laser beam or the irradiation of large ensem-
bles of nanostructures such as free-standing copper nanowires
grown in polymer ion-track membranes (Maurer et al 2006)
or nano-patterned arrays of doped silicon tips (Swanwick
et al 2014), possibly further enhanced by superradiance
effects. Very recently, the irradiation of blades has come into

24
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001
focus (Paschen et al 2018), enhancing the number of atoms in
the laser focus and potentially boosting HHG yield by a factor
of λ/R∼100.
10. Applications of tip-based photoemission
A wide range of applications of pulsed nanoscale electron
sources has been developed in the past ten years. Here, we
turn our attention first to applications that make direct use of
the sub-optical-cycle nature of the electron dynamics occur-
ring at the source itself (Section 10.1) and then extend our
scope to experiments and applications that employ the
coherent electron pulses subsequent to their generation
(section 10.2).
10.1. Lightwave metrology and control of electron dynamics in
time and space
The work presented in the previous chapters shows that the
photoemission and acceleration of electrons are field-driven
processes and can be controlled by the waveform of the
driving-laser field. This enables control of electric currents on
the attosecond time scale, opening up pathways towards
‘lightwave electronics’. Here, instead of a static field or a
microwave field in conventional electronics, an optical field
controls and steers electric currents at PHz frequencies
(Goulielmakis et al 2007, Krausz and Ivanov 2009, Krausz
and Stockman 2014) for which single-cycle optical pulses can
be achieved (Manzoni et al 2015, Hassan et al 2016). In order
to make use of the control capability, a nanoscale device is
necessary since the typical speed of an electron in a metal is
given by the Fermi velocity, which is of the order of nan-
ometer per femtosecond. Initial work towards a vacuum nano-
gap diode driven by a 5 fs, 800 nm laser pulse was performed
by Higuchi et al (2015), who approached two tungsten
nanotips with different radii to a distance of about 200 nm and
measured the photocurrent crossing the gap from the sharper
tip (serving as an anode) to the blunter tip (serving as a
cathode). The time resolution is of the order of hundreds of
femtoseconds corresponding to the gap crossing time. The
first sub-optical-cycle-resolved study of a laser-driven nano-
gap diode was performed by Rybka et al (2016). CEP-stable
6 fs pulses at a central wavelength of 1.3 μm were generated
and focused on a nano-gap antenna structure fabricated from
gold with electron-beam lithography (see figures 20(a) and
(b)). The gap was only 8 nm wide, which is why the
experiment could be performed in ambient air and at room
temperature. Scanning the CEP of the 1.4-cycle pulses leads
to the generation of a net current through the gap and also
influences its direction and magnitude. The mechanism here
is the strong dependence of tunneling photoemission on the
waveform of the pulse. Current pulses generated from half-
cycles with negative sign can exceed those generated from
half-cycles with positive sign and vice versa. It is the asym-
metric light field that breaks the symmetry and leads to a net
current flow. Waveform-induced forward-backward sym-
metry breaking can be enhanced by symmetry breaking of the
25
Topical Review
Figure 20. Lightwave electronics and coherent control of electric
currents. (a) Sketch of a lightwave-driven nano-gap antenna device
in air. The electric field F of a CEP-stable 6 fs laser pulse at 1.3 μm
(red and blue curves) drives a current I between two gold
nanoelectrodes separated by an 8 nm gap (inset: scanning electron
micrograph). The waveform asymmetry introduced by the CEP
determines the magnitude and direction of the current, which is
measured by a high-precision amperemeter. (b) Average current
expressed in pA and electrons per pulse as a function of the CEP (red
solid curve). The gray solid curves represent eight subsequent
measurements used for averaging. Waveforms corresponding to
three data points are indicated. Adapted by permission from
[Springer Nature]: [Nature Photonics] (Rybka et al 2016)), Nat.
Phot. 10. (c) Sketch of a coherent control experiment of above-
threshold photoemission from a tungsten nanotip using two colors
(1.55 μm and a weak admixture of its second harmonic). The
ω−2ω delay is the experimental control parameter. (d) Total
emission current as a function of sub-optical-cycle delay. The current
is modulated by up to 97.5%, corresponding to an almost perfect
switch-on-off scenario. Reprinted figure with permission from
Förster et al (2016), Copyright (2016) by the American Physical
Society. (e) Illustration of the underlying physical mechanism: two-
path quantum interference leads to a modulation of the total current.
A resonance located at an intermediate energy level (dashed line)
mediates the interference (EF: Fermi energy. Weff: Schottky-lowered
work function).
nano-electrode’s geometry. Putnam et al (2017) have reported
on an experiment where strong-field photoemission from
nanotriangle or nanorod arrays is triggered by 10 fs, 1.2 μm
pulses and detected by a large collector electrode at a distance
of about 5 μm. The authors find a detectable CEP-dependent
current only for the nanotriangle array since nanorods exhibit
forward-backward symmetry, while at nanotriangles a single
sharp feature contributes to the photoemission process. In the
latter case, only every other half-cycle produces photoelec-
trons, significantly enhancing CEP effects.
Symmetry breaking by the waveform of the light field
can also be achieved using two-color pulses. Working in the
multiphoton regime, Förster et al (2016), Paschen et al (2017)
and Seiffert et al (2018) used 74 fs, 1.55 μm pulses with a
weak admixture of the second harmonic and measured elec-
tron spectra and total current as a function of the two-color
delay (see figures 20(c)–(e)). They found strong sinusoidal
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001
oscillations of the total current with a periodicity of Topt/2
and a modulation depth of up to 97.5%. The experimental
results are consistent with two-path quantum interference
where one path includes the absorption of a second harmonic
photon and the other includes the absorption of two funda-
mental photons (see figure 20(e)). A DFT calculation revealed
a possible resonance in the SDOS, allowing for this type of
quantum path interference and a high degree of coherent
control. Another recent experiment explored the polarization
and delay dependence of multiphoton photoemission driven
by a two-color field (800 + 400 nm), but did not observe sub-
optical-cycle quantum interference (Huang et al 2017).
The waveform dependence of strong-field photoemission
and electron acceleration allows for the determination of the
CEP of ultrashort laser pulses. Nanotip experiments enable
CEP sensing, but for practical applications such as the sta-
bilization of the carrier-envelope offset frequency or single-
shot CEP measurements, the electron yield needs to be
increased by several orders of magnitude, for example by
using nanostructure arrays (Schenk et al 2011). The CEP of
the nano-optical near-field at a nanotip is shifted by a wave-
length- and geometry-dependent phase retardation with
respect to the CEP of the incident pulse (see section 2.2).
Therefore, spectrally resolved photocurrent measurements
enable measurements of the local CEP up to a constant phase
shift. Rescattered electrons are very sensitive to the CEP (see
Chapter 8). Strong-field photoemission from the apex of a
nanotip has been employed to measure the spatial variation of
the local CEP inside a focused broadband 4 fs laser pulse at a
wavelength of 700 nm as a function of longitudinal and radial
position. The focal phase does not follow the behavior of the
monochromatic Gouy phase, as one could naively assume,
but rather shows a strong dependence on the chromatic beam
properties, characterized to first order by the wavelength-
dependent Rayleigh range of the beam prior to focusing
(Porras 2009, Hoff et al 2017a, 2017b). The phase retardation
of the near-field with respect to the incident field has been
measured in a streaking experiment employing single isolated
attosecond XUV pulses (Förg et al 2016), implementing
attosecond nanoplasmonic streaking (Stockman et al 2007,
Süßmann and Kling 2011). Electrons released by XUV
photoemission are streaked by the near-field generated by an
ultrashort infrared pulse enabling its reconstruction.
Rescattered electrons also encode the strength of the light
field, which led to their creation and acceleration. For δ?1
(see Chapter 7), the rescattering cut-off encodes the intensity
of the near-field. Spectral measurements have been employed
to determine the near-field enhancement at nanotips (Thomas
et al 2013, Krüger et al 2014) and nanorod and bow-tie arrays
(Rácz et al 2017, 2018). For δ∼1, the near-field decay must
be taken into account, enabling a vectorial reconstruction of
the near-field (Park et al 2013). In addition to spectrally
resolved studies, measuring photoemission rates enables
rough estimates of the strength of the near-field, both in the
multiphoton regime (Ropers et al 2007c, Grubisic et al 2013)
and the transition regime to strong fields with its ‘kink’
around γ∼1.
26
Topical Review
Superimposing strong-field photoemission of a nanotip
with a low-frequency sub-two-cycle THz field adds a slowly
varying time-dependent electric field to the process (Herink
et al 2014, Wimmer et al 2014). Controlling the time delay
between the THz pulse and the strong infrared driving pulse
controls the kinetic energy distribution of the resulting elec-
tron pulse, which can be used to fully suppress photoemis-
sion. A systematic experimental and theoretical study
revealed the strong potential of spectro-temporal electron
pulse shaping using a combination of static and THz fields
(Wimmer et al 2017), in analogy to THz manipulation of free-
electron beams (Kealhofer et al 2016).
Most experiments described in this article are concerned
only with electron emission from the tip apex in the forward
direction, but the geometry and surface structure of a nanotip
allow manipulation of the spatial emission pattern by means
of laser polarization and incidence angle. Such manipulations
were reported by Yanagisawa et al (2009, 2010, 2013) for a
tungsten tip (R∼100 nm) in the photofield emission regime.
The interplay between the locally varying work function,
corresponding to different facets on the hemispherical tip
apex, and the local strength and direction of the near-field
enables a high degree of directional emission control. In
addition, emission from facets with low local work function
enables spatial double-slit experiments with polarization-
controlled fringe contrast (Yanagisawa et al 2017).
10.2. Laser-triggered nanotips as coherent source of electron
pulses
Pulsed coherent electron beams open up a wide range of
applications in ultrafast electron diffraction, microscopy and
matter-wave quantum optics. Nanotips are highly coherent
electron sources not only when operated in DC field emission
but also when triggered by ultrashort laser pulses. The virtual
source radius reff (also called effective source size) of a
nanotip is defined as the radius of a virtual incoherent emitter
that resembles the coherence properties of the tip. The smaller
reff, the more the tip acts like a (fully coherent) point source of
electrons. In DC field emission, reff can be in the order of
1 nm and even less for tips with radii of the order of 10 nm
(Spence 2013). The transverse coherence length is defined as
the size of coherent illumination of a sample by the electron
beam and is inversely proportional to reff. The coherence
properties of laser-triggered electron beams from a nanotip
were investigated for single-photon photoemission assisted by
the Schottky effect with kinetic energies in the order of 50 eV
(Ehberger et al 2015). Diffraction from a CNT placed close to
the nanotip was used to determine reff ; 0.8 nm for a tip
radius in the order of 10 nm, which compares well with reff ;
0.55 nm for DC field emission. The ratio K of transverse
coherence length to beam size was found to be 0.36—the
highest reported value for a laser-triggered electron source.
Comparable results have been found in an ultrafast trans-
mission electron microscope (UTEM) with a nanotip trig-
gered by two-photon photoemission (Feist et al 2017); at
200 keV electron energy, the authors find K≈0.11. Com-
pared to photocathode sources used for ultrafast electron
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001
microscopy (Reed et al 2009), nanotip emitters offer superior
coherence. Fully coherent femtosecond electron sources
might result from laser-driven single-atom tips. These tips end
in a single atom and are known to be fully coherent in DC
field emission operation (Fink 1986, Fu et al 2001, Hom-
melhoff et al 2009).
Laser-triggered nanotip-based electron guns require
electron optics to deliver the electrons on the sample. Point-
projection microscopy (PPM) is the simplest electron imaging
technique and relies on the nanometric size of the tip with
respect to a spatially resolving electron multiplier serving as a
screen (Fink et al 1990). A sample is placed very close (sub-
μm scale) to the tip and the electron trajectories emanating
from the tip apex lead to a magnification of the sample on the
screen of up to 106 allowing for ∼1 nm-resolution holo-
graphic imaging of single molecules in PPM (Longchamp
et al 2017). Several pioneering experiments explored imple-
mentations of time-resolved PPM using laser-triggered
nanotips (Quinonez et al 2013, Bainbridge et al 2016, Müller
et al 2016), with one experiment reporting the observation of
photo-excited currents in a nanowire with 50-fs resolution
(Müller et al 2015). At close tip-sample distances, it is
desirable to separate the optical excitation of the tip from that
of the sample. This can be achieved using grating-coupled
surface plasmon nanofocusing (Schröder et al 2015a,
Vogelsang et al 2015, Müller et al 2016) or a metal-coated
fiber tip (Casandruc et al 2015).
The integration of a laser-triggered nanotip into an
electron gun assembly usually requires a combination of a
suppressor electrode followed by acceleration and focusing
electron optics (Paarmann et al 2012, Hoffrogge et al 2014,
Bormann et al 2015, Storeck et al 2017). Due to matter-wave
dispersion of free electrons on the way to the sample, electron
pulse durations are limited to about 40 fs. Temporal electron
bunch compression to femtosecond durations, even up to the
formation of attosecond pulse trains, can be achieved through
interactions with microwave cavities, with near-fields at
nanostructures and material discontinuities in the THz and
optical domain (Kealhofer et al 2016, Hassan et al 2017,
Kozák et al 2017, Priebe et al 2017, Morimoto and
Baum 2018) and with the field of high-intensity optical tra-
veling waves (Kozák et al 2018a, 2018b). Sub-keV electron
pulses from nanotips have been applied for low-energy
electron diffraction (Gulde et al 2014, Müller et al 2015,
Storeck et al 2017, Vogelgesang et al 2018). The integration
of a laser-triggered nano-emitter has been demonstrated in a
scanning electron microscope (SEM) (Yang 2010, Kozák
et al 2018a) and in a UTEM reaching electron energies in
excess of 100 keV (Caruso et al 2017, Feist et al 2017,
Plemmons and Flannigan 2017, Houdellier et al 2018).
Nanotip photoemission is also explored for source
applications in electron accelerators because of its high-
brightness B. The brightness is defined as B = j (pbreff )2 ,
where β is the beam’s full opening angle and j is the total
emission current. A laser-triggered nanotip can serve as the
electron source in a multi-stage dielectric laser accelerator,
requiring high-brightness electron beams (Breuer and Hom-
melhoff 2013, Peralta et al 2013, England et al 2014, McNeur
27
Topical Review
et al 2016). In addition, conventional electron accelerators
benefit from high-brightness sources of electron bunches.
Fundamental emission mechanisms and beam properties of
nanostructure arrays were studied in order to increase the total
charge per electron bunch (see Mustonen et al 2011, Nagel
et al 2013, Keathley et al 2013, Vilayurganapathy et al 2013,
Swanwick et al 2014, Gubko et al 2014, Hobbs et al 2014,
Dong et al 2015, Li et al 2017).
Highly coherent electron pulses from nanotips also allow
for fundamental matter-wave quantum optics with free elec-
trons in the single-electron regime (see Jones et al (2016) for
a recent review). Notable is the test of the dispersionless
nature of the magnetic Aharonov–Bohm effect, adding a
time-dependent perspective to a basic quantum phenomenon
(Caprez et al 2007, Hilbert et al 2011, Batelaan and
Becker 2015). The interaction of nanotip-based UTEM elec-
tron pulses with nano-optical near-fields has enabled studies
of coherent manipulation and reconstruction of electron
quantum states (Feist et al 2015, Echternkamp et al 2016a,
Priebe et al 2017). Recently, ponderomotive acceleration of
an electron bunch in free space has been demonstrated with
the help of a laser-triggered SEM (Kozák et al 2018a, 2018b).
Finally, nanotips open up tests of Pauli degeneracy of free
electrons (Lougovski and Batelaan 2011, Jones et al 2016) as
the strong confinement of electron emission in time will lead
to much higher degeneracies than the record degeneracy of
10−4 achieved with a DC field emitter (Kiesel et al 2002).
11. Conclusion
Strong-field-driven photoemission from nanotips has been
developed into a powerful small-scale strong-field laboratory,
revealing for the first time fundamental attosecond phenom-
ena at the surface of nanoscale solids. The versatility of
nanotips has led to a wide variety of applications, with
ramifications in lightwave electronics and ultrafast material
science. Now the way is open to apply advanced methods of
attosecond spectroscopy to the nanoscale in order to study
ultrafast phenomena at surfaces and interfaces in real time.
We anticipate new and exciting research in the coming dec-
ade, enabled by the extreme localization of light and matter
on the (sub-) nanometer length and attosecond time scales.
12. List of symbols
• A(t): vector potential
• α: quiver radius
• β: electron beam full opening angle
• c, C: constants
• d: dipole moment
• D: density of states
• δ: dimensionless spatial adiabacity parameter
• δn: induced charge density change
• Δf: near-field phase shift
• Δθ: scattering angle
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001 Topical Review

• ΔWs: lowering of the surface-vacuum barrier by the • vF: Fermi velocity

Schottky effect • V: potential energy
• e: electron charge • Veff: effective potential
• Ecutoff: cut-off energy • Vext: external potential
• EF: Fermi energy • Vsurf: surface potential
• Ekin: kinetic energy • w: emission rate
• Ephot: photon energy • W: work function
• ò: dielectric function • Wi: electron binding energy
• ò0: dielectric constant • ξ: field enhancement factor
• f: prefactor to tunneling rates • z: reaction coordinate along surface normal
• fenv (t ): light field envelope function • zD: detector position
• F(t): time-dependent optical near-field
• F0: electric field amplitude
• FDC: DC field
• Feff: effective field amplitude including field enhancement 13. List of acronyms
• γ: Keldysh parameter
• 2PPE: two-photon photoemission
• ÿ: (reduced) Planck constant.
• APT: atom probe tomography
• I0: cycle-averaged peak intensity
• ATI: above-threshold ionization
• Ieff: effective cycle-averaged peak intensity including
• ATP: above-threshold photoemission
field enhancement
• BEM: boundary element method
• In: coefficients for the strong-field approximation
• CEP: carrier-envelope phase
• Ip: atomic ionization potential
• CNT: carbon nanotube
• j: electric current
• CTMC: classical trajectory Monte Carlo
• jFN: field emission current
• DFT: density functional theory
• k: wave number (electron or photon)
• SDOS: surface density of states
• kr: field reduction factor
• FDTD: finite-difference time-domain
• K: ratio of the transverse coherence length and electron-
• FN: Fowler and Nordheim
beam size
• FWHM: full width at half maximum
• lF: near-field decay constant
• HHG: high-harmonic generation
• λ: wavelength
• IR: infrared
• λF: Fermi wavelength
• LSP: localized surface plasmon
• λTF: Thomas–Fermi screening length
• MCP: micro-channel plate
• m: electron mass
• MPP: multiphoton photoemission
• nmin: minimum required number of photons to overcome
• OAP: off-axis parabolic mirror
the work function
• PPM: point-projection microscopy
• n(z, t): charge density
• SEM: scanning electron microscope
• ω: angular frequency
• SFA: strong-field approximation
• ωp: plasma frequency • SMMN: simple man’s model for nanotips
• Ω: solid emission angle
• SNOM: scanning near-field microscopy
• p: momentum
• TDDFT: time-dependent density functional theory
• P: electron spectrum
• TDSE: time-dependent Schrödinger equation
• fCE: carrier-envelope phase
• TERS: tip-enhanced Raman scattering
• fi: non-interacting pseudo-single-particle wavefunctions
• TOF: time of flight
• ψ: wavefunction
• UTEM: ultrafast transmission electron microscope
• ψd: direct wavepacket
• UV: ultraviolet
• ψr: rescattered wavepacket • VMI: velocity map imaging
• reff: effective source radius
• XUV: extreme ultraviolet
• R: tip radius of curvature
• S: action
• σp: width of momentum distribution
• t: time Acknowledgments
• t0: ionization time
• ts: recollision time MKand PHacknowledge funding through ERC Con-
• Topt optical-cycle duration solidator Grant ‘Near Field Atto’, DFG SFB 953, DFG SPP
• θ: tip half-opening angle 1840 ‘QUTIF’. CL, GWand JBthank the Austrian Science
• Θ: Heaviside function Fund (FWF), project numbers SFB-041 ViCoM, SFB-049
• Up: ponderomotive energy NextLite, and doctoral college W1243, and also the COST
• v: velocity Action CM1204 (XLIC) and the IMPRS-APS for support.

28
J. Phys. B: At. Mol. Opt. Phys. 51 (2018) 172001
Calculations were performed using the Vienna Scientific
Cluster (VSC). MKacknowledges financial support from the
Minerva Foundation and the Koshland Foundation.
ORCID iDs
Michael Krüger https://orcid.org/0000-0002-6188-9179
Christoph Lemell https://orcid.org/0000-0003-2560-4495
Peter Hommelhoff https://orcid.org/0000-0003-
4757-5410
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